Tetravalent Metal Phosphonate-Phosphate Hybrids as Catalyst Supports and Ion Exchange Materials
dc.contributor.advisor | Clearfield, Abraham | |
dc.contributor.advisor | Bluemel, Janet | |
dc.creator | Silbernagel, Rita Marie | |
dc.date.accessioned | 2020-02-27T20:13:32Z | |
dc.date.available | 2020-02-27T20:13:32Z | |
dc.date.created | 2016-05 | |
dc.date.issued | 2016-04-08 | |
dc.date.submitted | May 2016 | |
dc.identifier.uri | https://hdl.handle.net/1969.1/187417 | |
dc.description.abstract | This work centers on recycling of Rh catalysts and utilizing ion exchange to separate nuclear waste. In the area of Rh-type catalyst supports, non-porous zirconium phosphate nanoplatelets (ZrP) were utilized to provide sufficient outside surface area while still being easily separable from the reaction mixtures. First, a phosphine linker containing an ethoxysilyl group, (EtO)3Si(CH2)3PPh2, is reacted with ZrP. Addition of Wilkinson's catalyst ClRh(PPh3)3 to the phosphine-modified ZrP gives the immobilized catalyst. In the absence of pore diffusion, the catalytic hydrogenation of 1-dodecene using the Rhtype immobilized catalyst proceeds with unprecedented speed and the catalyst can be recovered and recycled 15 times. New materials were synthesized that are comprised of Zr/Sn phosphonate-phosphate hybrids. The general formula for these materials is M(O3PC6H4PO3)1-x/2(APO4)x•nH2O, where M = Zr^4+, Sn^4+; A = H, Na, K; and x = 0, 0.5, 0.8, 1.0, 1.33, 1.6. These materials have a preference for ions of high charge (3+, 4+) over those with lower charge (1+, 2+). From this charge-based affinity and pH modification, separations can be achieved with Nd^3+/Cs^+ separation factors ≥ 100. The stability of these materials to 3.18 MGy gamma radiation was also observed with performance and structure retained. Greater than 99% removal of radioactive Am(III) from solution was obtained. Similar materials have also been utilized to explore rare earth recovery from Compact Fluorescent Lamps and Cr(VI) removal from wastewater solutions. | en |
dc.format.mimetype | application/pdf | |
dc.language.iso | en | |
dc.subject | chemistry | en |
dc.subject | zirconium phosphate | en |
dc.subject | zirconium phosphonate | en |
dc.subject | tin phosphonate | en |
dc.subject | ion exchange | en |
dc.subject | immobilized catalyst | en |
dc.subject | Wilkinson's Catalyst | en |
dc.subject | nanoparticles | en |
dc.subject | Cr(VI) | en |
dc.subject | ion exchange | en |
dc.subject | rare earth recovery | en |
dc.subject | green chemistry | en |
dc.subject | en | |
dc.title | Tetravalent Metal Phosphonate-Phosphate Hybrids as Catalyst Supports and Ion Exchange Materials | en |
dc.type | Thesis | en |
thesis.degree.department | Chemistry | en |
thesis.degree.discipline | Chemistry | en |
thesis.degree.grantor | Texas A&M University | en |
thesis.degree.name | Doctor of Philosophy | en |
thesis.degree.level | Doctoral | en |
dc.contributor.committeeMember | Folden III, Charles M | |
dc.contributor.committeeMember | Ozerov, Oleg | |
dc.type.material | text | en |
dc.date.updated | 2020-02-27T20:13:32Z | |
local.etdauthor.orcid | 0000-0002-0547-7313 |
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