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f-block MOFs: A Pathway to Heterometallic Transuranics.
Park, Kyoung Chul; Kittikhunnatham, Preecha; Lim, Jaewoong; Thaggard, Grace C; Liu, Yuan; Martin, Corey R; Leith, Gabrielle A; Toler, Donald J; Ta, An T; Birkner, Nancy; Lehman-Andino, Ingrid; Hernandez-Jimenez, Alejandra; Morrison, Gregory; Amoroso, Jake W; Zur Loye, Hans-Conrad; DiPrete, Dave P; Smith, Mark D; Brinkman, Kyle S; Phillpot, Simon R; Shustova, Natalia B.
Affiliation
  • Park KC; Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208, USA.
  • Kittikhunnatham P; Department of Chemistry, Chulalongkorn University, Bangkok, 10330, Thailand.
  • Lim J; Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208, USA.
  • Thaggard GC; Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208, USA.
  • Liu Y; Department of Materials Science and Engineering, University of Florida, Gainesville, FL 32611, USA.
  • Martin CR; Savannah River National Laboratory, Aiken, SC 29808, USA.
  • Leith GA; Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208, USA.
  • Toler DJ; Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208, USA.
  • Ta AT; Department of Materials Science and Engineering, University of Florida, Gainesville, FL 32611, USA.
  • Birkner N; Department of Materials Science and Engineering, Clemson University, Clemson, SC 29634, USA.
  • Lehman-Andino I; Center for Nuclear Environmental Engineering Sciences and Radioactive Waste Management (NEESRWM), Clemson University, Clemson, SC 29634, USA.
  • Hernandez-Jimenez A; Savannah River National Laboratory, Aiken, SC 29808, USA.
  • Morrison G; Savannah River National Laboratory, Aiken, SC 29808, USA.
  • Amoroso JW; Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208, USA.
  • Zur Loye HC; Savannah River National Laboratory, Aiken, SC 29808, USA.
  • DiPrete DP; Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208, USA.
  • Smith MD; Savannah River National Laboratory, Aiken, SC 29808, USA.
  • Brinkman KS; Savannah River National Laboratory, Aiken, SC 29808, USA.
  • Phillpot SR; Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208, USA.
  • Shustova NB; Department of Materials Science and Engineering, Clemson University, Clemson, SC 29634, USA.
Angew Chem Int Ed Engl ; 62(5): e202216349, 2023 Jan 26.
Article in En | MEDLINE | ID: mdl-36450099
ABSTRACT
A novel series of heterometallic f-block-frameworks including the first examples of transuranic heterometallic 238 U/239 Pu-metal-organic frameworks (MOFs) and a novel monometallic 239 Pu-analog are reported. In combination with theoretical calculations, we probed the kinetics and thermodynamics of heterometallic actinide(An)-MOF formation and reported the first value of a U-to-Th transmetallation rate. We concluded that formation of uranyl species could be a driving force for solid-state metathesis. Density of states near the Fermi edge, enthalpy of formation, band gap, proton affinity, and thermal/chemical stability were probed as a function of metal ratios. Furthermore, we achieved 97 % of the theoretical maximum capacity for An-integration. These studies shed light on fundamental aspects of actinide chemistry and also foreshadow avenues for the development of emerging classes of An-containing materials, including radioisotope thermoelectric generators or metalloradiopharmaceuticals.
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Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: Angew Chem Int Ed Engl Year: 2023 Document type: Article Affiliation country: Estados Unidos
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Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: Angew Chem Int Ed Engl Year: 2023 Document type: Article Affiliation country: Estados Unidos