Local Environment of Terbium(III) Ions in Layered Nanocrystalline Zirconium(IV) Phosphonate–Phosphate Ion Exchange Materials
The structures of Zr(IV) phosphonate-phosphate based, unconventional metal organic framework materials have been determined using atomic pair distribution function analysis of high energy, X-ray total scattering diffraction data. They are found to form as nanocrystalline layers of Zr phosphate, sim...
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| Published in | Inorganic chemistry Vol. 56; no. 15; pp. 8837 - 8846 |
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| Main Authors | , , , , |
| Format | Journal Article |
| Language | English |
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United States
American Chemical Society
07.08.2017
American Chemical Society (ACS) |
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| Abstract | The structures of Zr(IV) phosphonate-phosphate based, unconventional metal organic framework materials have been determined using atomic pair distribution function analysis of high energy, X-ray total scattering diffraction data. They are found to form as nanocrystalline layers of Zr phosphate, similar to the bulk, but with a high degree of interlayer disorder and intermediate intralayer order extending around 5 nm. These materials are of interest for their high selectivity for 3+ lanthanide ions. To investigate the mechanism of the selectivity, we utilize difference pair distribution function analysis to extract the local structural environment of Tb3+ ions loaded into the framework. The ions are found to sit between the layers in a manner resembling the local environment of Tb in Scheelite-type terbium phosphate. By mapping this local structure onto that of the refined structure for zirconium-phenyl-phosphonate, we show how dangling oxygens from the phosphate groups, acting like nose hairs, are able to reorient to provide a friendly intercalation environment for the Tb3+ ions. |
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| AbstractList | The structures of Zr(IV) phosphonate-phosphate based, unconventional metal organic framework materials have been determined using atomic pair distribution function analysis of high energy, X-ray total scattering diffraction data. They are found to form as nanocrystalline layers of Zr phosphate, similar to the bulk, but with a high degree of interlayer disorder and intermediate intralayer order extending around 5 nm. These materials are of interest for their high selectivity for 3+ lanthanide ions. To investigate the mechanism of the selectivity, we utilize difference pair distribution function analysis to extract the local structural environment of Tb3+ ions loaded into the framework. The ions are found to sit between the layers in a manner resembling the local environment of Tb in Scheelite-type terbium phosphate. By mapping this local structure onto that of the refined structure for zirconium-phenyl-phosphonate, we show how dangling oxygens from the phosphate groups, acting like nose hairs, are able to reorient to provide a friendly intercalation environment for the Tb3+ ions. The structures of Zr(IV) phosphonate-phosphate based, unconventional metal organic framework materials have been determined using atomic pair distribution function analysis of high energy, X-ray total scattering diffraction data. They are found to form as nanocrystalline layers of Zr phosphate, similar to the bulk, but with a high degree of interlayer disorder and intermediate intralayer order extending around 5 nm. These materials are of interest for their high selectivity for 3+ lanthanide ions. To investigate the mechanism of the selectivity, we utilize difference pair distribution function analysis to extract the local structural environment of Tb3+ ions loaded into the framework. The ions are found to sit between the layers in a manner resembling the local environment of Tb in Scheelite-type terbium phosphate. By mapping this local structure onto that of the refined structure for zirconium-phenyl-phosphonate, we show how dangling oxygens from the phosphate groups, acting like nose hairs, are able to reorient to provide a friendly intercalation environment for the Tb3+ ions.The structures of Zr(IV) phosphonate-phosphate based, unconventional metal organic framework materials have been determined using atomic pair distribution function analysis of high energy, X-ray total scattering diffraction data. They are found to form as nanocrystalline layers of Zr phosphate, similar to the bulk, but with a high degree of interlayer disorder and intermediate intralayer order extending around 5 nm. These materials are of interest for their high selectivity for 3+ lanthanide ions. To investigate the mechanism of the selectivity, we utilize difference pair distribution function analysis to extract the local structural environment of Tb3+ ions loaded into the framework. The ions are found to sit between the layers in a manner resembling the local environment of Tb in Scheelite-type terbium phosphate. By mapping this local structure onto that of the refined structure for zirconium-phenyl-phosphonate, we show how dangling oxygens from the phosphate groups, acting like nose hairs, are able to reorient to provide a friendly intercalation environment for the Tb3+ ions. Not provided. The structures of Zr(IV) phosphonate-phosphate based, unconventional metal organic framework materials have been determined using atomic pair distribution function analysis of high energy, X-ray total scattering diffraction data. They are found to form as nanocrystalline layers of Zr phosphate, similar to the bulk, but with a high degree of interlayer disorder and intermediate intralayer order extending around 5 nm. These materials are of interest for their high selectivity for 3+ lanthanide ions. To investigate the mechanism of the selectivity, we utilize difference pair distribution function analysis to extract the local structural environment of Tb ions loaded into the framework. The ions are found to sit between the layers in a manner resembling the local environment of Tb in Scheelite-type terbium phosphate. By mapping this local structure onto that of the refined structure for zirconium-phenyl-phosphonate, we show how dangling oxygens from the phosphate groups, acting like nose hairs, are able to reorient to provide a friendly intercalation environment for the Tb ions. |
| Author | Shi, Chenyang Terban, Maxwell W Silbernagel, Rita Clearfield, Abraham Billinge, Simon J. L |
| AuthorAffiliation | Department of Chemistry Columbia University Condensed Matter Physics and Materials Science Department Department of Applied Physics and Applied Mathematics Texas A&M University Brookhaven National Laboratory |
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| Author_xml | – sequence: 1 givenname: Maxwell W orcidid: 0000-0002-7094-1266 surname: Terban fullname: Terban, Maxwell W organization: Columbia University – sequence: 2 givenname: Chenyang orcidid: 0000-0002-2291-7325 surname: Shi fullname: Shi, Chenyang organization: Columbia University – sequence: 3 givenname: Rita surname: Silbernagel fullname: Silbernagel, Rita organization: Texas A&M University – sequence: 4 givenname: Abraham orcidid: 0000-0001-8318-8122 surname: Clearfield fullname: Clearfield, Abraham organization: Texas A&M University – sequence: 5 givenname: Simon J. L surname: Billinge fullname: Billinge, Simon J. L email: sb2896@columbia.edu organization: Brookhaven National Laboratory |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/28704045$$D View this record in MEDLINE/PubMed https://www.osti.gov/biblio/1534539$$D View this record in Osti.gov |
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| Title | Local Environment of Terbium(III) Ions in Layered Nanocrystalline Zirconium(IV) Phosphonate–Phosphate Ion Exchange Materials |
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