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Characterization of surface-bound Zr(IV) and its application to removal of As(V) and As(III) from aqueous systems using phosphonic acid modified nanoporous silica polyamine composites / Varadharajan Kailasam in Industrial & engineering chemistry research, Vol. 48 N° 8 (Avril 2009) 

Public ISBD [article]  in Industrial & engineering chemistry research > Vol. 48 N° 8 (Avril 2009) . - pp. 3991–4001 Titre : Characterization of surface-bound Zr(IV) and its application to removal of As(V) and As(III) from aqueous systems using phosphonic acid modified nanoporous silica polyamine composites Type de document : texte imprimé Auteurs : Varadharajan Kailasam, Auteur ; Edward Rosenberg, Auteur ; Daniel Nielsen, Auteur Année de publication : 2009 Article en page(s) : pp. 3991–4001 Note générale : Chemical engineering Langues : Anglais (eng) Mots-clés : Silica  polyamine  composites  Phosphonic  acid  modified  composite  Mannich  reaction Résumé : Silica polyamine composites (SPC) made from silanized amorphous nanoporous silica gel and poly(allylamine) (BP-1) were functionalized with phosphorus acid using the Mannich reaction, resulting in a phosphonic acid modified composite (BPAP). Successful immobilization of the phosphonic acid ligand was confirmed by mass gain, elemental analysis, IR, and solid-state NMR. The modified composite had a ligand loading of 1.5 mmol/g, corresponding to N/P ratio of 0.73. Zirconium(IV) was immobilized on BPAP with a loading of 1.12 mmol/g. Zirconium loading was analyzed by mass gain, ICP/AES, and SEM/EDX. Arsenate anions strongly adsorbed on the ZrBPAP composite in the pH range 2−8, while arsenite only adsorbed well at pH 10. The sorption mechanism is a chelation between arsenate or arsenite and Zr(IV)−phosphonic acid complex of BPAP. Adsorption isotherm data were found to be well modeled by the Langmuir equation for As(V) at pH 4 with Kads = 0.016 L/g and Qm = 98 mg/g; and at pH 6 with Kads = 0.018 L/g and Qm = 56 mg/g. Regeneration of the resin was carried out successfully for As(V) and As(III) using 2M-H2SO4. Four adsorption/desorption cycles were performed for As(V) at pH 4 without significant decrease in the uptake performance. ZrBPAP capture capacity and kinetics for arsenate were tested for longevity over 1000 cycles with only a marginal loss of performance. This composite is highly selective for arsenate over sulfate (As/SO42− = 50/1) and selenate (As/Se = 20/1); lower selectivity was observed with Fe(III) and Th(IV) loaded BPAP. The significance of the observed selectivity is discussed in terms of the chemical properties of the anion and the nature of the interactions with the immobilized metal site. En ligne : http://pubs.acs.org/doi/abs/10.1021/ie8016362 [article] Characterization of surface-bound Zr(IV) and its application to removal of As(V) and As(III) from aqueous systems using phosphonic acid modified nanoporous silica polyamine composites [texte imprimé] / Varadharajan Kailasam, Auteur ; Edward Rosenberg, Auteur ; Daniel Nielsen, Auteur . - 2009 . - pp. 3991–4001. Chemical engineering Langues : Anglais (eng) in Industrial & engineering chemistry research > Vol. 48 N° 8 (Avril 2009) . - pp. 3991–4001 Mots-clés : Silica  polyamine  composites  Phosphonic  acid  modified  composite  Mannich  reaction Résumé : Silica polyamine composites (SPC) made from silanized amorphous nanoporous silica gel and poly(allylamine) (BP-1) were functionalized with phosphorus acid using the Mannich reaction, resulting in a phosphonic acid modified composite (BPAP). Successful immobilization of the phosphonic acid ligand was confirmed by mass gain, elemental analysis, IR, and solid-state NMR. The modified composite had a ligand loading of 1.5 mmol/g, corresponding to N/P ratio of 0.73. Zirconium(IV) was immobilized on BPAP with a loading of 1.12 mmol/g. Zirconium loading was analyzed by mass gain, ICP/AES, and SEM/EDX. Arsenate anions strongly adsorbed on the ZrBPAP composite in the pH range 2−8, while arsenite only adsorbed well at pH 10. The sorption mechanism is a chelation between arsenate or arsenite and Zr(IV)−phosphonic acid complex of BPAP. Adsorption isotherm data were found to be well modeled by the Langmuir equation for As(V) at pH 4 with Kads = 0.016 L/g and Qm = 98 mg/g; and at pH 6 with Kads = 0.018 L/g and Qm = 56 mg/g. Regeneration of the resin was carried out successfully for As(V) and As(III) using 2M-H2SO4. Four adsorption/desorption cycles were performed for As(V) at pH 4 without significant decrease in the uptake performance. ZrBPAP capture capacity and kinetics for arsenate were tested for longevity over 1000 cycles with only a marginal loss of performance. This composite is highly selective for arsenate over sulfate (As/SO42− = 50/1) and selenate (As/Se = 20/1); lower selectivity was observed with Fe(III) and Th(IV) loaded BPAP. The significance of the observed selectivity is discussed in terms of the chemical properties of the anion and the nature of the interactions with the immobilized metal site. En ligne : http://pubs.acs.org/doi/abs/10.1021/ie8016362

Polymer structure and metal ion selectivity in silica polyamine composites modified with sodium chloroacetate and nitriloacetic acid (NTA) anhydride / Mark A. Hughes in Industrial & engineering chemistry research, Vol. 47 N°17 (Septembre 2008) 

Public ISBD [article]  in Industrial & engineering chemistry research > Vol. 47 N°17 (Septembre 2008) . - p. 6765–6774 Titre : Polymer structure and metal ion selectivity in silica polyamine composites modified with sodium chloroacetate and nitriloacetic acid (NTA) anhydride Type de document : texte imprimé Auteurs : Mark A. Hughes, Auteur ; Jessica Wood, Auteur ; Edward Rosenberg, Auteur Année de publication : 2008 Article en page(s) : p. 6765–6774 Note générale : Chemical engineering Langues : Anglais (eng) Mots-clés : Silica  polyamine  composite  Amine  ligands Résumé : Previously, silica polyamine composite (SPC) materials (BP-1 and WP-1) containing amine chelating groups were prepared using two polyamines, polyallylamine (PAA), and polyethyleneimine (PEI). In this paper the amine ligands of BP-1 and WP-1 were modified with chloroacetate, yielding the new SPC materials BP-2 and WP-2. We have found that the acetate groups were bound to the amine groups to a greater extent on the SPC prepared using PAA (BP-1) relative to the SPC prepared with PEI (WP-1). BP-2 was selective for Cu2+ over other divalent metal ions from polymetallic solutions in the pH range of 1 to 3. In contrast, WP-2 was selective for Cu2+ over other divalent metal ions at pH 1 only and coloaded significant amounts of Ni2+ at pH 2 and pH 3. Thus, polyamine structure impacts the metal selectivity of the resultant SPC materials, BP-2 and WP-2. Two novel SPCs were prepared from nitriloacetic acid (NTA) anhydride using BP-1 and WP-1, yielding BP-NT and WP-NT, respectively. The resultant materials possess a unique chelating ligand, in which an iminodiacetic acid (IDA) group is covalently bonded to the SPC amine groups via an amide bond. The two materials (BP-NT, WP-NT) have similar metal selectivity profiles indicating that polyamine structure is not influential. Increased ligand denticity and the amide linker prevent the polymer from playing a large role in selectivity. The resulting materials have the ability to remove divalent and trivalent metal ions from low pH aqueous solutions. These materials can be regenerated by treatment with acid solution and showed no evidence of amide bond hydrolysis under acidic conditions. En ligne : http://pubs.acs.org/doi/abs/10.1021/ie800359k [article] Polymer structure and metal ion selectivity in silica polyamine composites modified with sodium chloroacetate and nitriloacetic acid (NTA) anhydride [texte imprimé] / Mark A. Hughes, Auteur ; Jessica Wood, Auteur ; Edward Rosenberg, Auteur . - 2008 . - p. 6765–6774. Chemical engineering Langues : Anglais (eng) in Industrial & engineering chemistry research > Vol. 47 N°17 (Septembre 2008) . - p. 6765–6774 Mots-clés : Silica  polyamine  composite  Amine  ligands Résumé : Previously, silica polyamine composite (SPC) materials (BP-1 and WP-1) containing amine chelating groups were prepared using two polyamines, polyallylamine (PAA), and polyethyleneimine (PEI). In this paper the amine ligands of BP-1 and WP-1 were modified with chloroacetate, yielding the new SPC materials BP-2 and WP-2. We have found that the acetate groups were bound to the amine groups to a greater extent on the SPC prepared using PAA (BP-1) relative to the SPC prepared with PEI (WP-1). BP-2 was selective for Cu2+ over other divalent metal ions from polymetallic solutions in the pH range of 1 to 3. In contrast, WP-2 was selective for Cu2+ over other divalent metal ions at pH 1 only and coloaded significant amounts of Ni2+ at pH 2 and pH 3. Thus, polyamine structure impacts the metal selectivity of the resultant SPC materials, BP-2 and WP-2. Two novel SPCs were prepared from nitriloacetic acid (NTA) anhydride using BP-1 and WP-1, yielding BP-NT and WP-NT, respectively. The resultant materials possess a unique chelating ligand, in which an iminodiacetic acid (IDA) group is covalently bonded to the SPC amine groups via an amide bond. The two materials (BP-NT, WP-NT) have similar metal selectivity profiles indicating that polyamine structure is not influential. Increased ligand denticity and the amide linker prevent the polymer from playing a large role in selectivity. The resulting materials have the ability to remove divalent and trivalent metal ions from low pH aqueous solutions. These materials can be regenerated by treatment with acid solution and showed no evidence of amide bond hydrolysis under acidic conditions. En ligne : http://pubs.acs.org/doi/abs/10.1021/ie800359k