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PubMed2005

Adsorption mechanism of synthetic reactive dye wastewater by chitosan.

Chitosan was able to remove the color from synthetic reactive dye wastewater (SRDW) under acidic and caustic conditions. The effect of the initial pH on SRDW indicated that electrostatic interaction occurred between the effective functional groups (amino groups) and the dye under acidic conditions. Moreover, SRDW adsorption under caustic conditions was also affected by the covalent bonding of dye and hydroxyl groups of chitosan. In addition, elution tests confirmed that chemical adsorption occurred under acidic conditions, while both physical and chemical adsorption appeared under caustic conditions. The spectra of attenuated total reflectance Fourier transform infrared spectrometry confirmed the functional groups of chitosan that affected the SRDW adsorption. However, the maximum adsorption capacities of chitosan increased when the temperature increased. The maximum adsorption capacity of chitosan obtained from the Langmuir model was 68, 110, and 156 mg g(-1) under a system pH of 11.0 at 20, 40, and 60 degrees C, respectively. The negative values of enthalpy change (DeltaH), free energy change (DeltaG), and entropy change (DeltaS) indicated an exothermic, spontaneous process and decreasing disorder of the system, respectively. Therefore, the mechanism of SRDW adsorption by chitosan was probably by chemical adsorption for a wide range of pH's and at high temperatures.

Journal Article↗
PubMed2005

Competitive adsorption of organic matter with phosphate on aluminum hydroxide.

The effects of orthophosphate on the adsorption of natural organic matter (NOM) on aluminum hydroxide were investigated using three organic compounds as surrogates, including humic acid (HA), phthalic acid, and 2,3-dihydroxybenzoic acid (2,3-DHBA). The adsorption of phthalic acid and 2,3-DHBA was very limited compared to that of HA, whereas their adsorption was reduced much more significantly than that of HA by phosphate. The efficiency of phosphate in reducing HA adsorption increased with increasing phosphate concentration. Phosphate adsorption was slightly reduced by phthalic acid and 2,3-DHBA but moderately suppressed by HA. The adjacent carboxylic groups mainly contributed to the adsorption of humic acid at low pH, while the adjacent phenol groups were responsible for the adsorption of humic acid at high pH. HPLC-SEC and SUVA analysis revealed that HA molecules with high molecular weight were adsorbed preferentially but were easily displaced by the specifically adsorbed phosphate. TM-AFM images revealed that the aggregation of HA molecules and the protonation of carboxylic groups at low pH facilitated the adsorption under acidic conditions. The presence of phosphate increases the coagulant dosage for NOM removal as some sites on the coagulant precipitates become utilized by phosphate.

Journal Article↗
PubMed2006

Adsorption of guar gum onto quartz from dilute mixed electrolyte solutions.

The effect of potassium, sodium, calcium, magnesium, and hydrogen cations on adsorption of guar gum onto quartz was investigated at natural pH. The role of the background ions was analyzed in terms of their water-structure making or breaking capabilities. In dilute solutions (0.01 mol/L) of structure-makers (NaCl, HCl, CaCl2, and MgCl2), the guar gum adsorption density did not change compared to the adsorption densities obtained in distilled water. Potassium, the only structure-breaking ion (chaotrope) among the tested cations, significantly enhanced guar gum adsorption. The results obtained in mixed electrolytes demonstrate that the strong structure-breaking properties of K+ overcome any contributions from weak structure making ions (kosmotropes), and guar gum adsorption remains at the levels observed in KCl alone. Only when strongly hydrated Mg2+ ions are mixed with KCl, the overall effect becomes additive and the influence of potassium is proportionally reduced by increasing concentrations of magnesium cations. In this approach, guar gum adsorption on quartz is viewed as a competition between polysaccharide and water molecules for silanol surface sites. The hydration of the quartz surface inhibits the adsorption process but the competition equilibrium, and hence polysaccharide adsorption, can be affected by the presence of chaotropes or kosmotropes.

Journal Article↗
PubMed2006

A novel and simple method for finding the heterogeneity of adsorbents on the basis of adsorption kinetic data.

The heterogeneity of adsorbent was characterized by a novel and simple method that uses adsorption kinetic data from solution. On the basis of different simulated adsorption kinetic data for heterogeneous adsorbents with two different adsorption sites, it was found that there is a deviation from linearity in pseudo-second-order adsorption kinetic models. The patterns of obtained diagrams (t/qt vs t) shows five main classes of adsorption. On the basis of this novel and simple method it is possible to show that the surface of adsorbents is homogeneous or heterogeneous, and in the case of heterogeneous surfaces it is possible to find the differences between adsorption sites. For finding kinetic constants of adsorption on heterogeneous surfaces with two different sites, a new equation was presented and called the two-site pseudo-second-order (TS-PSO) model. Finally, some experimental kinetic data of adsorption were analyzed by the new method.

Journal Article↗
PubMed2006

Kinetic and isothermal studies of lead ion adsorption onto palygorskite clay.

The use of a natural palygorskite clay for the removal of Pb(II) from aqueous solutions for different contact times, pHs of suspension, and amounts and particle sizes of palygorskite clay were investigated. The variations of the pH value of Pb(II) solutions on natural palygorskite in the adsorption process were determined. Batch adsorption kinetic experiments revealed that the adsorption of Pb(II) onto palygorskite clay involved fast and slow processes. It was found that the adsorption mechanisms in the lead/palygorskite system follow pseudo-second-order kinetics with a significant contribution from film diffusion. SEM observations demonstrated that an important interaction at the lead-granule interface occurred during the adsorption process. The adsorption isotherms were described by means of the Langmuir and Freundlich isotherms and the Langmuir model represents the adsorption process better than the Freundlich model. The maximum adsorption capacity of Pb(II) onto natural palygorskite was 104.28 mg g(-1).

Journal Article↗
PubMed2005

Determination of the equilibrium, kinetic and thermodynamic parameters of adsorption of copper(II) ions onto seeds of Capsicum annuum.

Adsorption of copper ions onto Capsicum annuum (red pepper) seeds was investigated with the variation in the parameters of pH, contact time, adsorbent and copper(II) concentrations and temperature. The nature of the possible adsorbent and metal ion interactions was examined by the FTIR technique. The copper(II) adsorption equilibrium was attained within 60 min. Adsorption of copper(II) ions onto C. annuum seeds followed by the Langmuir, Freundlich and Dubinin-Radushkevich (D-R) isotherm models. Maximum adsorption capacity (q(max)) of copper(II) ions onto red pepper seeds was 4.47x10(-4) molg(-1) at 50 degrees C. Three kinetic models including the pseudo-first-order, pseudo-second-order and intraparticle diffusion equations were selected to follow the adsorption process. Kinetic parameters such as rate constants, equilibrium adsorption capacities and related correlation coefficients, for each kinetic model were calculated and discussed. It was indicated that the adsorption of copper(II) ions onto C. annuum seeds could be described by the pseudo-second-order kinetic model and also followed the intraparticle diffusion model up to 60 min, but diffusion is not only the rate controlling step. Thermodynamics parameters such as the change of free energy, enthalpy and entropy were also evaluated for the adsorption of copper(II) ions onto C. annuum seeds.

Capsicum↗
PubMed2002

Calorimetric effects accompanying ion adsorption at the charged metal oxide/electrolyte interfaces: effects of the correlations between the binding-to-surface energies of various surface complexes.

As has been shown in our earlier publications, a theoretical description of ion adsorption at the real, energetically heterogeneous oxide/electrolyte interfaces, involves necessary assumption about the correlations between the adsorption energies of the various surface complexes formed at this interface. So far, only two extreme models have been considered in such theoretical descriptions: one model assuming that high correlations exist, and the other assuming that practically no correlations exist. The purpose of this paper is to develop yet another description based on a model assuming that some partial correlations exist between the adsorption energies of the various surface complexes. The other purpose of this publication is to test these three models by analysing some experimental data reported so far in literature. Such data sets must include necessary information about the enthalpic effects accompanying ion adsorption. This is because enthalpic effects are known to be more sensitive to the mechanistic models underlying a theoretical description of adsorption systems. With such requirements in mind, we have selected three adsorption systems: Al2O3/NaCl, TiO2/NaCl and silica/NaCl, for our analysis. Our theoretical-numerical analysis of the behaviour of these adsorption systems suggests that either none or partial correlations exist between the adsorption energies of the various surface complexes. However, that analysis also shows, that the present accuracy of the experimental data does not allow us to draw more elaborate conclusions.

Journal Article↗
PubMed2003

Behaviors and mechanisms of copper adsorption on hydrolyzed polyacrylonitrile fibers.

Polyacrylonitrile fiber (PANF) was hydrolyzed in a solution of sodium hydroxide and the hydrolyzed polyacrylonitrile fiber (HPANF) was used as an adsorbent to remove copper ions from aqueous solution. Scanning electron microscopy (SEM) showed that the hydrolysis process made the surface of HPANF rougher than that of PANF. Fourier transform infrared (FTIR) spectroscopy revealed that the HPANF contained conjugated imine (-Cz=Nz-) sequences. Batch adsorption results indicated that the HPANF was very effective in adsorbing copper, and the adsorption equilibrium could be reached within 10-20 min. Atomic force microscopy (AFM) showed that some aggregates formed on the surface of the HPANF after copper ion adsorption and the average surface roughness (R(a)) value of the HPANF changed from 0.363 to 3.763 nm due to copper adsorption. FTIR analysis indicated that copper adsorption caused a decrease of the light adsorption intensity of the imine (-Cz=Nz-) groups at 1573 and 1406 cm(-1) wavenumbers, and X-ray photoelectron spectroscopy (XPS) showed that the binding energy (BE) of some of the nitrogen atoms in the HPANF increased to a greater value due to copper adsorption. The FTIR and XPS results suggest that the adsorption of copper ions to the HPANF is attributed to the imine groups on the surface of the HPANF.

Journal Article↗
PubMed2004

Adsorption of Co, Ni, Cu, and Zn on hydrous manganese dioxide from complex electrolyte solutions resembling sea water in major ion content.

Adsorption of Co, Ni, Cu, and Zn onto a poorly crystalline hydrous manganese dioxide (delta-MnO2) has been studied in complex electrolyte solutions such as (a) 0.5 M NaCl+0.054 M MgCl2, (b) 0.5 M NaCl+0.028 M Na2SO4, and (c) artificial sea water prepared according to the standard literature method. These three solutions allow us to identify the specific effect of major cations, major anions, and the mixture of major cations and anions (including carbonate and bicarbonate) that is present in real sea water. The adsorption isotherm in major ion sea water at pH 7.25 indicates that while Co and Zn exhibit increases in adsorption with increase in concentration, Ni shows relatively poor adsorption, reaching a plateau at 0.075 mM concentration. The three trace metals (Co, Ni, and Zn) show Langmuirian behavior for adsorption at low concentration. It is generally observed that the fractional adsorption vs pH curve shifts to higher pH either in the presence of 0.054 M MgCl2 or in sea water. In the presence of 0.028 M Na2SO4 the fractional adsorption vs pH curve remains almost unchanged with respect to a 0.5 M NaCl solution. The competitive adsorption of one trace metal in the presence of other three in major ion sea water indicates that this phenomenon is more predominant with Ni and Zn than with Co and Cu.

Journal Article↗
PubMed2003

The influence of chain length and electrolyte on the adsorption kinetics of cationic surfactants at the silica-aqueous solution interface.

The equilibrium and kinetic aspects of the adsorption of alkyltrimethylammonium surfactants at the silica-aqueous solution interface have been investigated using optical reflectometry. The effect of added electrolyte, the length of the hydrocarbon chain, and of the counter- and co-ions has been elucidated. Increasing the length of the surfactant hydrocarbon chain results in the adsorption isotherm being displaced to lower concentrations. The adsorption kinetics indicate that above the cmc micelles are adsorbing directly to the surface and that as the chain length increases the hydrophobicity of the surfactant has a greater influence on the adsoption kinetics. While the addition of 10 mM KBr increases the CTAB maximal surface excess, there is no corresponding increase for the addition of 10 mM KCl to the CTAC system. This is attributed to the decreased binding efficiency of the chloride ion relative to the bromide ion. Variations in the co-ion species (Li, Na, K) have little effect on the adsorption rate and surface excess of CTAC up to a bulk electrolyte concentration of 10 mM. However, the rate of adsorption is increased in the presence of electrolyte. Slow secondary adsorption is seen over a range of concentrations for CTAC in the absence of electrolyte and importantly in the presence of LiCl; the origin of this slow adsorption is attributed to a structural barrier to adsorption.

Journal Article↗
PubMed2003

An infrared study of CO adsorption on silica-supported Ru-Sn catalysts.

CO adsorption on Ru-Sn/SiO(2) catalysts of various Sn/(Ru+Sn) ratios was examined by Diffuse Reflectance Infrared Fourier-Transform Spectroscopy (DRIFTS). The catalysts were prepared by the incipient wetness impregnation method. Catalysts were activated by H(2) reduction at 773 K. CO adsorbed on the catalysts shows spectra whose band frequencies are divided into three groups: (i) High Frequency Region (HFR), containing a band at 2065 cm(-1), (ii) Low Frequency Region 1 (LFR(1)), containing bands at 2040-2015 cm(-1), (iii) Low Frequency Region 2 (LFR(2)), containing bands at 1990 and 1945 cm(-1). The types of adsorbed CO species formed strongly depend on the ratio Sn/(Ru+Sn) in the catalyst, CO pressure and temperature of adsorption. Adsorption of CO on Ru sites in the Ru/SiO(2) catalyst results in LFR(1) bands at 2040-2015 cm(-1), which are independent of the CO pressure but the adsorption complexes are easily destroyed by raising the temperature. The addition of Sn to the catalyst creates new sites for CO adsorption. After adsorption at 298 K, the HFR band at 2065 cm(-1) and LFR(2) bands at 1990-1950 cm(-1) are observed. The relative intensities of these bands increase with increasing Sn-content in the samples. The LFR bands are thermally stable while the HFR band is not. The formation of the corresponding species is favored by increasing the CO pressure. Adsorbed CO species giving LFR(1) bands are assigned to linearly-adsorbed CO on the Ru(0) and/or on the Ru-Sn alloy sites. Adsorbed CO species giving HFR bands are assigned to CO adsorption on Ru(delta+)-O-Sn sites. After low temperature CO adsorption on samples with high Sn-content, only species that show bands at 1990 and 1945 cm(-1) in LFR(2) are observed.

Carbon Monoxide↗
PubMed1998

Production of cell-free xanthan fermentation broth by cell adsorption on fibers

Xanthan gum is a microbial polysaccharide widely used in food and oil-drilling industries. Xanthan gum produced from the current commercial fermentation process usually contains cells and cell debris, which lower the filterability of the xanthan solution and limit its applications. The production of cell-free xanthan gum fermentation broth is thus desirable. The feasibility of removing cells from the xanthan fermentation broth by cell adsorption to various woven fibrous materials was studied. It was found that both cotton and polyester fibers could be used to adsorb Xanthomonas campestris cells present in the fermentation broth either during batch fermentation or after the fermentation. Almost all cells were removed from the fermentation broth by adsorption to fibers. Cotton terry cloth had rough surfaces and was the preferred material for cell adsorption. Cell adsorption to cotton was faster than to polyester fibers. The adsorption kinetics can be modeled by a first-order rate equation. The adsorption rate constants were 30-40% higher for cotton than for polyester. Cell adsorption was not efficient in the absence of xanthan gum, suggesting that the exopolysaccharide, xanthan gum, was important for efficient cell adsorption to fibers.

Journal Article↗
PubMed2005

Adsorption of atomic hydrogen at a nanostructured electrode of polyacrylate-capped Pt nanoparticles in polyelectrolyte.

Atomic hydrogen electrosorption is reported at crystallite sites of polyacrylate-capped Pt nanoparticles (d = 2.5 +/- 0.6 nm), by assembling nanostructured electrodes of polyacrylate-Pt nanocrystallites layer-by-layer in a cationic polyelectrolyte, poly(diallyldimethylammonium chloride). Cyclic voltammetry in 1 M H2SO4 revealed a strongly adsorbed hydrogen state and a weakly adsorbed hydrogen state assigned to adsorption at (100) and (110) sites of the modified nanocrystallites, respectively. Resolving hydrogen adsorption states signifies that surface capping by the carboxylate groups is not irreversibly blocking hydrogen adsorption sites at the modified Pt nanoparticle surface. Adsorption peak currents increased with increasing the number of layers up to 16 bilayers, indicating the feasibility of nanoparticle charging via interparticle charge hopping and the accessibility of adsorption states within the thickness of the nanoparticle/polyelectrolyte multilayers. Despite similarity in hydrogen adsorption in the cyclic voltammorgrams in 1 M H2SO4, negative shifts in adsorption potentials were measured at the nanocrystallite Pt-polyelectrolyte multilayers relative to a polycrystalline bulk Pt surface. This potential shift is attributed to a kinetic limitation in the reductive hydrogen adsorption as a result of the Pt nanoparticle surface modification and the polyelectrolyte environment.

Absorption↗
PubMed2005

Cluster and periodic DFT calculations: the adsorption of atomic nitrogen on M(111) (M = Cu, Ag, Au) surfaces.

First-principle density functional calculations with cluster and slab models have been performed to investigate adsorption and thermally activated atomic nitrogen on M(111) (M = Cu, Ag, Au) surfaces. Optimized results indicate that the basis set of the N atom has a distinct effect on the adsorption energy but an indistinct one on the equilibrium distance. For the N/M(111) adsorption systems studied here, the threefold face centered cubic (fcc) hollow site is found to be the most stable adsorption site. The reason for the fcc site is that the perfected adsorption site has been explained by the density of states (DOS) analysis, that is, that N(2p) has the smallest DOS population near the Fermi level on the fcc site as compared with other adsorption sites. The variations of the adsorption energy as a function of adsorption site are similar and in the following order of N-M(111) binding strengths on a given site: Cu(111) > Ag(111) > Au(111). It is found that the N atom forms essentially an ionic bond for the most stable site. Large contributions between the M(ns) and N(2p) orbitals (n = 4, 5, and 6 for Cu, Ag, and Au, respectively) are found for the cluster model at the B3LYP/LANL2DZ-6-31G(d,p) level and also found in the slab DFT-GGA calculation results, which are the main characteristics of M-N bonds. At last, the dissociation of N2 on Cu(111) and Au(111) has also been obtained in this work, and the results showed that the dissociation of N2 on Cu(111) is more active than that on the Au(111) surface.

Journal Article↗
PubMed2006

On the difficulties of predicting the adsorption of volatile organic compounds at low pressures in microporous solid: the example of ethyl benzene.

Adsorption isotherms of toluene and ethyl benzene, at 25 degrees C and 40 degrees C, were determined in two microporous activated carbons and one zeolite. Significant differences were found in the adsorption behavior, at low pressures, between the two vapors on the same adsorbent material. The quantities of adsorbed ethyl benzene at 25 degrees C, in the low-pressure region, were lower than what was observed at 40 degrees C in all the studied adsorbents, contrary to what was found for toluene. This fact was not related to kinetic effects at the two temperatures nor to vapor swelling of the adsorbents structure. Also, there was no molecular sieving since at high pressures the toluene and ethyl benzene occupied the same adsorption space. The differences found in the ethyl benzene adsorption at the two temperatures pose difficulties in the analysis of the adsorption data and, therefore, in the prediction of results. This is discussed in the analysis of the results with the application of the Dubinin-Astakhov equation and in the estimation of the isosteric heats of adsorption. The adsorption potentials of two possible ethyl benzene conformations were estimated for the adsorption in the pores of activated carbon from the Horvath and Kawazoe model, and the values compared with those found experimentally. The results were interpreted in terms of the ethyl benzene conformation effects when the molecule is confined in pores that are about the same size of one of the conformations.

Journal Article↗
PubMed2006

Theoretical and experimental investigation of morphology and temperature effects on adsorption of organic vapors in single-walled carbon nanotubes.

Hexane adsorption on single-walled carbon nanotube (SWNT) bundles is studied by both simulation and experimentally using a previously developed computer-aided methodology, which employed a smaller physisorbed probe molecule, nitrogen, to explore the porosity of nanotube samples. Configurational-bias grand canonical Monte Carlo simulation of hexane adsorption on localized sites of the bundles is carried out to predict adsorption on their external surface and in their internal sites. These localized isotherms are then combined into a global isotherm for a given sample by using knowledge of its tube-diameter distribution and structural parameters, such as the fraction of open-ended nanotubes and the external surface area of bundles in samples, which have been independently determined from the standard nitrogen adsorption isotherm. The near-perfect replication of experimental isotherms demonstrates the validity of our method for structural characterization of SWNT samples. The effect of temperature on adsorption is also studied and the simulation results are extrapolated to predict the limiting hexane adsorption capacity of the samples. The similarity between the hexane adsorption isotherms and those of other organic molecules demonstrates that the adsorption mechanisms explored here are not specific to hexane, and that the proposed methodology can be potentially applicable to other sorbates with equal success.

Journal Article↗
PubMed2006

Adsorption and photophysics of fullerene C60 at liquid-zeolite particle interfaces: unusually high affinity for hydrophobic, ultrastabilized zeolite Y.

Adsorption of fullerene C60 from solution to the external surface of zeolite particles has been investigated. The most intriguing result of this study was the nature of C60 adsorption to ultrastablized zeolite Y (or USY). Two commercial samples of USY were tested: CBV780 (Y780) and CBV901 (Y901). Y901 was shown in previous reports to be more hydrophobic than Y780. Higher affinity of C60 for Y901 was found relative to Y780 in a variety of hydrocarbon solvents, including toluene and cyclohexane. In these same solvents, weak or no affinity for Y901 of typical arenes such as naphthalene or pyrene was observed. In toluene, adsorption isotherms for C60 gave dissociation constants (and values of saturation binding) = 0.5 microM (5.8 micromol g(-1)) and 8 microM (1.4 micromol g(-1)) for Y901 and Y780, respectively. C60 was estimated to cover nearly one-half of the estimated external surface area of Y901 particles at saturation. Significant adsorption of C60 to the ionic zeolites NaX, NaY, and KL was observed in cyclohexane but not in toluene, consistent with the pi-cation effect as a driving force for adsorption to these materials. The main driving force for C60 adsorption to Y901 is postulated to involve the interaction of C60 with lone pair electrons of framework oxygen atoms of the 12-ring entry aperture to the supercage. In the 12-ring site, C60 is located in half-supercage bowls on the exterior particle surface. The adsorptive interaction on Y901 relies on the spherical shape of C60 and the hydrophobicity of the zeolite surface. On ionic zeolites, the presence of specific adsorption sites such as exchangeable cations and hydroxyl groups hinder the special positioning necessary for C60 interaction with the 12-ring site. The ground-state and triplet-state absorption spectrum of adsorbed C60 was solution-like on all zeolites. Quenching of the C60 triplet state was examined by using transient absorption spectroscopy. Rate constants for quenching by rubrene, ferrocene, and O2 at the Y901-toluene interface were 18, 9, and 3 times lower, respectively, relative to rate constants in solution. These differences point out that the approach of molecular quenchers to C60 at the interface is more hindered for larger molecules, an expected result for C60 located in half-supercage bowls. The high affinity of fullerenes for hydrophobic zeolite Y provides a strategy for organizing fullerenes at interfaces and for studies of fullerene photochemistry.

Journal Article↗
PubMed2006

Adsorption kinetics of NIPAM-based polymers at the air-water interface as studied by pendant drop and bubble tensiometry.

The adsorption of N-isopropylacrylamide (NIPAM) based thermoresponsive polymers at the air-water interface was investigated by using drop and bubble shape tensiometry. The molecular weight dependence of polymer adsorption rate was studied by using narrowly distributed polymer fractions (polydispersity < 1.2) that were prepared by solvent:nonsolvent fractionation. The time-dependent surface tension profiles were fitted to the Hua-Rosen equation and the t values obtained were applied for interpretation of the kinetic data. It was found that the rate of polymer adsorption increased as the molecular weight of the polymer decreased. The relationship between polymer surface concentration and surface tension was determined by applying the pendant drop as a Langmuir-type film balance. From this relationship, the kinetics of polymer adsorption determined experimentally was compared with the adsorption rates predicted by a diffusion-controlled adsorption model based on the Ward-Tordai equation. The predicted adsorption rates were in good agreement with what was found experimentally. The dependence of the adsorption rate on the molecular weight of polymers can be satisfactorily described within the diffusion-controlled model.

Journal Article↗