Hybrid inorganic-organic adsorbents, Part 1: synthesis and characterization of mesoporous zirconium titanate frameworks containing coordinating organic functionalities

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dc.contributor.authorGriffith, CSen_AU
dc.contributor.authorReyes, MDLen_AU
dc.contributor.authorScales, Nen_AU
dc.contributor.authorHanna, JVen_AU
dc.contributor.authorLuca, Ven_AU
dc.date.accessioned2011-01-18T03:15:54Zen_AU
dc.date.available2011-01-18T03:15:54Zen_AU
dc.date.issued2010-12-22en_AU
dc.date.statistics2010-12-22en_AU
dc.description.abstractA series of functional hybrid inorganic−organic adsorbent materials have been prepared through postsynthetic grafting of mesoporous zirconium titanate xerogel powders using a range of synthesized and commercial mono-, bis-, and tris-phosphonic acids, many of which have never before been investigated for the preparation of hybrid phases. The hybrid materials have been characterized using thermogravimetric analysis, diffuse reflectance infrared (DRIFT) and 31P MAS NMR spectroscopic techniques and their adsorption properties studied using a 153Gd radiotracer. The highest level of surface functionalization (molecules/nm2) was observed for methylphosphonic acid (3 molecules/nm2). The level of functionalization decreased with an increase in the number of potential surface coordinating groups of the phosphonic acids. Spectral decomposition of the DRIFT and 31P MAS NMR spectra showed that each of the phosphonic acid molecules coordinated strongly to the metal oxide surface but that for the 1,1-bis-phosphonic acids and tris-phosphonic acids the coordination was highly variable resulting in a proportion of free or loosely coordinated phosphonic acid groups. Functionalization of a porous mixed metal oxide framework with the tris-methylenephosphonic acid (ATMP-ZrTi-0.33) resulted in a hybrid with the highest affinity for 153Gd3+ in nitric acid solutions across a wide range of acid concentrations. The ATMP-ZrTi-0.33 hybrid material extracted 153Gd3+ with a Kd value of 1 × 104 in 0.01 M HNO3 far exceeding that of the other hybrid phases. The unfunctionalized mesoporous mixed metal oxide had negligible affinity for Gd3+ (Kd < 100) under identical experimental conditions. It has been shown that the presence of free or loosely coordinated phosphonic acid groups does not necessarily translate to affinity for 153Gd3+. The theoretical cation exchange capacity of the ATMP-ZrTi-0.33 hybrid phase for Gd3+ has been determined to be about 0.005 mmol/g in 0.01 M HNO3. This behavior and that of the other hybrid phases suggests that the surface-bound ATMP ligand functions as a chelating ligand toward 153Gd3+ under these acidic conditions. © 2010, American Chemical Societyen_AU
dc.identifier.citationGriffith, C. S., Reyes, M. D. L., Scales, N., Hanna, J. V., & Luca, V. (2010). Hybrid inorganic−organic adsorbents, Part 1: synthesis and characterization of mesoporous zirconium titanate frameworks containing coordinating organic functionalities. ACS Applied Materials & Interfaces, 2(12), 3436-3446. doi:10.1021/am100891uen_AU
dc.identifier.govdoc3133en_AU
dc.identifier.issn1944-8244en_AU
dc.identifier.issue12en_AU
dc.identifier.journaltitleACS Applied Materials & Interfacesen_AU
dc.identifier.pagination3436-3446en_AU
dc.identifier.urihttp://dx.doi.org/10.1021/am100891uen_AU
dc.identifier.urihttp://apo.ansto.gov.au/dspace/handle/10238/2934en_AU
dc.identifier.volume2en_AU
dc.language.isoenen_AU
dc.publisherAmerican Chemical Societyen_AU
dc.subjectZirconiumen_AU
dc.subjectAdsorbentsen_AU
dc.subjectHybridizationen_AU
dc.subjectNuclear magnetic resonanceen_AU
dc.subjectOrganic acidsen_AU
dc.subjectIsotopesen_AU
dc.titleHybrid inorganic-organic adsorbents, Part 1: synthesis and characterization of mesoporous zirconium titanate frameworks containing coordinating organic functionalitiesen_AU
dc.typeJournal Articleen_AU
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