Effect of the presence of Fe (0) on the sorption of lanthanum and lutetium mixtures in smectites

The sorption of La and Lu mixtures was examined in two bentonites after incubation for three months at 20 and 80 °C with Fe(0), as a laboratory approach to evaluate the effects of waste canister corrosion in a deep repository on the performance of clay engineered barriers. The sorption/desorption parameters were determined from batch tests in two ionic media: deionized water and, to consider the additional effect of cement leachates, 0.02 mol L− 1 Ca. Results from XRD analyses showed the formation of crystalline FeO(OH), goethite, in a few samples and the degradation of the bentonites due to Fe(0) oxidation during incubation. Moreover, the EDX spectra showed that the lanthanides were sorbed primarily at smectite sites, although sorption onto goethite was also observed, whereas Fe(0) particles did not contribute to lanthanide sorption. The formation of goethite could explain the high Kd values measured in a few scenarios (e.g., those with single solutions or mixtures with the lowest initial concentration of the competitive lanthanide in which high affinity sites governed sorption), with up to 3-fold increases over the values obtained without Fe incubation. However, at higher lanthanide concentration, Kd values decreased or remained constant compared to the samples without Fe incubation, which could be explained by bentonite degradation. In the Ca medium, as much as 5 times lower Kd values were obtained, because of the competitive effect of the Ca ions, especially for Lu in the MX80 bentonite. This indicated that the small number of high affinity sites had been diminished. The sorption data were satisfactorily fitted to a two-solute Langmuir model. In addition, Kd values correlated well with desorption data, which showed that the larger the decrease in Kd, the larger the increase in sorption reversibility. It is suggested that corrosion products from the metal canister might compromise the long-term radionuclide retention of the clay-engineered barriers.Peer Reviewe

Examination of competitive lanthanide sorption onto smectites and its significance in the management of radioactive waste

The competitive effect of La and Lu (analogues of radionuclides appearing in radioactive waste) in the sorption in four smectites was examined. Sorption and desorption distribution coefficients (Kd; Kd,des), and desorption rates (Rdes) were determined from batch tests in two media: deionized water and, to consider the influence of cement leachates, 0.02molL-1 Ca. The competitive effect was lower when high-affinity sites were available, as in the water medium at the lowest range of initial lanthanide concentration, with high Kd for La and for Lu (5-63×104Lkg-1). Lower Kd was measured at higher initial concentrations and in the Ca medium, where Lu showed a stronger competitive effect. This was confirmed by fitting the sorption data to a two-solute Langmuir isotherm. The desorption data indicated that sorption was virtually irreversible for the scenarios with high sorption, with an excellent correlation between Kd and Kd,des (R2 around 0.9 for the two lanthanides). Assuming that radioactive waste is a mixture of radionuclides, and that Ca ions will be provided by the cement leachates, this would reduce the retention capacity of clay engineered barriers. © 2010 Elsevier B.V.This research was supported by grants from the Ministry of Education and Science of Spain (Ministerio de Educación y Ciencia de España) for the Project CTM2008-01147/TECNO, from DGICYT for the Project CTQ2007-63297, and from EC for the Project funded within the 6th Framework Programme as the HRM Activity under the Contract MRTN-CT-2006-035957. Besides, the authors would like to thank Dr. A. Padró for his technical help and assistance in the ICP-OES and ICP-MS analyses. SEM-EDX analyses were carried out at the Instituto Ciencia de los Materiales de Sevilla (CICIC).  Peer Reviewe

3-mercaptopropyltrimethoxysilane-modified Multi-walled Carbon Nanotubes As A New Functional Adsorbent For Flow Injection Extraction Of Pb(ii) From Water And Sediment Samples

In the present study, a novel synthesized adsorbent material based on 3-mercaptopropyltrimethoxysilanefunctionalized multi-walled carbon nanotubes was used to increase the Pb2+ adsorption from aqueous solutions in a flow injection solid-phase extraction system coupled to flame atomic absorption spectrometry. Spectroscopic and microscopic techniques (Fourier transform infrared spectroscopy, energy dispersive spectroscopy, and scanning electronmicroscopy) were employed to confirm the chemical modification of the adsorbent surface. Preconcentration conditions (sample pH, flow rate, buffer solution, and eluent concentrations) were optimized using factorial and Doehlert matrix designs that made it possible to construct a linear graph in the 5.0- to 130.0-μgL-1 range (r0 0.9999) and estimate detection and quantification limits (1.7 and 5.7 μgL-1, respectively). The method precision was found to be 4.20 and 1.97%for 5.0 and 100.0 μgL -1 Pb2+ solutions, respectively. When using the 3-mercaptopropyltrimethoxysilane-functionalized multiwalled carbon nanotubes, the sensitivity for the Pb2+ trace determination was improved to 95 % compared with the oxidized multi-walled carbon nanotubes, thus evidencing the significant enhancement of the adsorption capacity. The developed method was successfully applied to the analysis of Pb2+ species in different water samples and the PACS-2 marine sediment-certified reference material. © Springer Science+Business Media Dordrecht 2012.223960696081Afzali, D., Mostafavi, A., Potential of modified multiwalled carbon nanotubes with 1-(2-pyridylazo)-naphthol as a new solid sorbent for the preconcentration of trace amounts of cobalt(II) ion (2008) Analytical Sciences, 24, pp. 1135-1139Afzali, D., Jamshidi, R., Ghaseminezhad, S., Afzali, Z., Preconcentration procedure trace amounts of palladium using multiwalled carbon nanotubes sorbent prior to flame atomic absorption spectrometry (2012) Arabian Journal of Chemistry, 5, pp. 461-466Aviles, F., Cauich-Rodriguez, J.V., Moo-Tah, L., May-Pat, A., Vargas-Coronado, R., Evaluation of mild acid oxidation treatments for MWCNT functionalization (2009) Carbon, 47, pp. 2970-2975Barbosa, A.F., Segatelli, M.G., Pereira, A.C., Santos, A.S., Kubota, L.T., Luccas, P.O., Solid-phase extraction system for Pb(II) ions enrichment based on multiwall carbon nanotubes coupled on-line to flame atomic spectrometry (2007) Talanta, 71, pp. 1512-1519Narsito Nuryono, B., Kunarti, E.S., Production of metal ion imprinted polymer from mercapto-silica through sol-gel process as selective adsorbent of cadmium (2010) Desalination, 251, pp. 83-89Cai, Y., Jiang, G., Liu, J., Zhou, Q., Multiwalled carbon nanotubes as a solid-phase extraction adsorbent for the determination of bisphenol A, 4-nnonylphenol, and 4-tert-octylphenol (2003) Analytical Chemistry, 75, pp. 2517-2521Cheng, H., Hu, Y., Lead (Pb) isotopic fingerprinting and its applications in lead pollution studies in China: A review (2010) Environmental Pollution, 158, pp. 1134-1146(2005) CONAMA - National Council for the Environment, , http://www.mma.gov.br/port/conama/legiabre.cfm?codlegi0459, Resolução CONAMA No 357. 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419-430Needleman, H., Lead poisoning (2004) Annual Review of Medicine, 55, pp. 209-222Ren, X., Shao, D., Zhao, G., Sheng, G., Hu, J., Yang, S., Wang, X., Plasma induced multiwalled carbon nanotube grafted with 2-vinylpyridine for preconcentration of Pb(II) fromaqueous solutions (2011) Plasma Process Polymer, 8, pp. 589-598Sandroni, V., Smith, C.M.M., Donovan, A., Microwave digestion of sediment, soils and urban particulate matter for trace metal analysis (2003) Talanta, 60, pp. 715-723Savio, M., Parodi, B., Martinez, L.D., Smichowski, P., Gil, R.A., On-line solid-phase extraction of Ni and Pb using carbon nanotubes and modified carbon nanotubes coupled to ETAAS (2011) Talanta, 85, pp. 245-251Shamspur, T., Mostafavi, A., Application of modified multiwalled carbon nanotubes as a sorbent for simultaneous separation and preconcentration trace amounts of Au(III) and Mn(II) (2009) Journal of Hazardous Materials, 168, pp. 1548-1553Soylak, M., Tuzen, M., Diaion SP-850 resin as a new solid 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3-mercaptopropyltrimethoxysilane-Modified Multi-walled Carbon Nanotubes as a New Functional Adsorbent for Flow Injection Extraction of Pb(II) from Water and Sediment Samples

Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)In the present study, a novel synthesized adsorbent material based on 3-mercaptopropyltrimethoxysilane-functionalized multi-walled carbon nanotubes was used to increase the Pb2+ adsorption from aqueous solutions in a flow injection solid-phase extraction system coupled to flame atomic absorption spectrometry. Spectroscopic and microscopic techniques (Fourier transform infrared spectroscopy, energy dispersive spectroscopy, and scanning electronmicroscopy) were employed to confirm the chemical modification of the adsorbent surface. Preconcentration conditions (sample pH, flow rate, buffer solution, and eluent concentrations) were optimized using factorial and Doehlert matrix designs that made it possible to construct a linear graph in the 5.0- to 130.0-mu gL(-1) range (r=0.9999) and estimate detection and quantification limits (1.7 and 5.7 mu gL(-1), respectively). The method precision was found to be 4.20 and 1.97% for 5.0 and 100.0 mu gL(-1) Pb2+ solutions, respectively. When using the 3-mercaptopropyltrimethoxysilane-functionalized multi-walled carbon nanotubes, the sensitivity for the Pb2+ trace determination was improved to 95 % compared with the oxidized multi-walled carbon nanotubes, thus evidencing the significant enhancement of the adsorption capacity. The developed method was successfully applied to the analysis of Pb2+ species in different water samples and the PACS-2 marine sediment-certified reference material.223960696081Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)Instituto Nacional de Ciencia e Tecnologia de Bioanalitica (INCT)Fundacao Araucaria do ParanaFAEPE-UELConselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES

Synthesis Of Novel Copper Ion-selective Material Based On Hierarchically Imprinted Cross-linked Poly(acrylamide-co-ethylene Glycol Dimethacrylate)

A novel hierarchically imprinted cross-linked poly(acrylamide-co-ethylene glycol dimethacrylate) using a double-imprinting approach for the Cu 2+ selective separation from aqueous medium was prepared. In the imprinting process, both Cu2+ ions and surfactant micelles (cetyltrimethylammonium bromide - CTAB) were employed as templates. The hierarchically imprinted organic polymer named (IIP-CTAB), single-imprinted (IIP-no CTAB) and non-imprinted (NIP-CTAB and NIP-no CTAB) polymers were characterized by SEM, FTIR, TG, elemental analysis and textural data from BET (Brunauer-Emmett-Teller) and BJH (Barrett-Joyner-Halenda). Compared to these materials, IIP-CTAB showed higher selectivity, specific surface area and adsorption capacity toward Cu2+ ions. Good selectivity for Cu 2+ was obtained for the Cu2+/Cd2+, Cu 2+/Zn2+ and Cu2+/Co2+ systems when IIP-CTAB was compared to the single-imprinted (IIP-no CTAB) and non double-imprinted polymer (NIP-CTAB), thereby confirming the improvement in the polymer selectivity due to double-imprinting effect. For adsorption kinetic data, the best fit was provided with the pseudo-second-order model for the four materials, thereby indicating the chemical nature of the Cu2+ adsorption process. Cu2+ adsorption under equilibrium was found to follow dual-site Langmuir-Freundlich model isotherm, thus suggesting the existence of adsorption sites with low and high binding energy on the adsorbent surface. From column experiments 600 adsorption-desorption cycles using 1.8 mol L-1 HNO3 as eluent confirmed the great recoverability of adsorbent. 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Kinetic And Isotherm Studies Of Ni2+adsorption On Poly(methacrylic Acid) Synthesized Through A Hierarchical Double-imprinting Method Using A Ni2+ Ion And Cationic Surfactant As Templates

A novel poly(methacrylic acid) material (IIP/CTAB) was prepared by a hierarchical double-imprinting process with Ni2+ ion and cationic surfactant - cetyltrimethylammonium bromide (CTAB) as templates, and it was employed to adsorb Ni2+ ions from aqueous medium. Other poly(methacrylic acid) materials - single-imprinted (IIP/no CTAB) and nonimprinted (NIP/no CTAB) were investigated in adsorption studies. All the synthesized polymers were characterized by FTIR, SEM, and nitrogen adsorption-desorption isotherm. The maximum Ni2+ adsorption capacities of IIP/CTAB and NIP/no CTAB were found to be 33.31 and 18.64 mg g-1, respectively, at pH 7.25. The relative selectivity coefficient (k′) values for Ni2+/Cu2+, Ni2+/Mn +, Ni2+/Co2+ and Ni2+/Pb 2+ systems were higher than 1, thus confirming the significant improvement in the selectivity of the polymer. 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