Hydrolytic stability of mesoporous zirconium titanate frameworks containing coordinating organic functionalities

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dc.contributor.authorde los Reyes, Men_AU
dc.contributor.authorMajewski, PJen_AU
dc.contributor.authorScales, Nen_AU
dc.contributor.authorLuca, Ven_AU
dc.date.accessioned2015-09-29T02:10:28Zen_AU
dc.date.available2015-09-29T02:10:28Zen_AU
dc.date.issued2013-04-12en_AU
dc.date.statistics2015-09-18en_AU
dc.description.abstractThe hydrolytic stability of lanthanide and actinide selective mono- and polyphosphonate-functionalized mesoporous zirconium titanium oxide adsorbents has been investigated in nitric acid solutions. Hydrolytic degradation of the surfaces, as measured through the fractional loss of phosphorus and elements of the oxide framework, increased by more than an order of magnitude as the nitric acid concentration was increased from 0 to 2 mol/L. The unfunctionalized parent oxide suffered considerable dissolution in 2 mol/L acid over a period of 72 h. Under identical conditions, the fractional Zr and Ti release was reduced to 1 × 10–2 for monophosphonate functionalized hybrids and reached as low as 1 × 10–6 for trisphosphonate functionalized variants. The bisphosphonates showed intermediate values. The leaching of P, Zr and Ti was found to be incongruent with the Zr leaching to a lesser extent implying enhanced stability of the Zr–O–P bond. Quantitative analysis of the dissolution kinetics indicated a parabolic dissolution model with a rate constant in the range of 0.5–1.5 mg g–1 min–1/2 for the elemental leaching of P, Ti, and Zr. The leaching of Zr from the mesoporous matrix was relatively more complex than for the other elements with evidence of a leaching mechanism involving two processes. ToF-SIMS and DRIFT analysis demonstrated that after leaching in 2 M HNO3 for 24 h, a significant proportion of grafted ligands remained on the surface. The oxide functionalized with amino trismethylenephosphonic acid, which had previously shown excellent 153Gd3+ selectivity, was demonstrated to have outstanding stability, with low fractional elemental losses and preservation of mesoporous texture even after leaching for 24 h in 2 M HNO3. This suggests this particular hybrid to be worthy of additional study. © 2013, American Chemical Society.en_AU
dc.identifier.citationde los Reyes, M., Majewski, P. J., Scales, N., & Luca, V. (2013). Hydrolytic Stability of mesoporous zirconium titanate frameworks containing coordinating organic functionalities. ACS Applied Materials & Interfaces, 5(10), 4120-4128. doi:10.1021/am3031695en_AU
dc.identifier.govdoc6091en_AU
dc.identifier.issn1944-8244en_AU
dc.identifier.issue10en_AU
dc.identifier.journaltitleACS Applied Materials & Interfacesen_AU
dc.identifier.pagination4120-4128en_AU
dc.identifier.urihttp://dx.doi.org/10.1021/am3031695en_AU
dc.identifier.urihttp://apo.ansto.gov.au/dspace/handle/10238/6243en_AU
dc.identifier.volume5en_AU
dc.language.isoenen_AU
dc.publisherAmerican Chemical Societyen_AU
dc.subjectZirconiumen_AU
dc.subjectTitaniumen_AU
dc.subjectPhosphonic acidsen_AU
dc.subjectPhosphonatesen_AU
dc.subjectLeachingen_AU
dc.subjectNitric aciden_AU
dc.titleHydrolytic stability of mesoporous zirconium titanate frameworks containing coordinating organic functionalitiesen_AU
dc.typeJournal Articleen_AU
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