f-block MOFs: A Pathway to Heterometallic Transuranics
Kyoung Chul Park
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorProf. Dr. Preecha Kittikhunnatham
Department of Chemistry, Chulalongkorn University, Bangkok, 10330 Thailand
Search for more papers by this authorDr. Jaewoong Lim
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorGrace C. Thaggard
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorYuan Liu
Department of Materials Science and Engineering, University of Florida, Gainesville, FL 32611 USA
Search for more papers by this authorDr. Corey R. Martin
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorDr. Gabrielle A. Leith
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorDonald J. Toler
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorDr. An T. Ta
Department of Materials Science and Engineering, University of Florida, Gainesville, FL 32611 USA
Search for more papers by this authorDr. Nancy Birkner
Department of Materials Science and Engineering, Clemson University, Clemson, SC 29634 USA
Center for Nuclear Environmental Engineering Sciences and Radioactive Waste Management (NEESRWM), Clemson University, Clemson, SC 29634 USA
Search for more papers by this authorDr. Ingrid Lehman-Andino
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorDr. Alejandra Hernandez-Jimenez
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorDr. Gregory Morrison
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorDr. Jake W. Amoroso
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorProf. Dr. Hans-Conrad zur Loye
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorDr. Dave P. DiPrete
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorDr. Mark D. Smith
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorProf. Dr. Kyle S. Brinkman
Department of Materials Science and Engineering, Clemson University, Clemson, SC 29634 USA
Center for Nuclear Environmental Engineering Sciences and Radioactive Waste Management (NEESRWM), Clemson University, Clemson, SC 29634 USA
Search for more papers by this authorProf. Dr. Simon R. Phillpot
Department of Materials Science and Engineering, University of Florida, Gainesville, FL 32611 USA
Search for more papers by this authorCorresponding Author
Prof. Dr. Natalia B. Shustova
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorKyoung Chul Park
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorProf. Dr. Preecha Kittikhunnatham
Department of Chemistry, Chulalongkorn University, Bangkok, 10330 Thailand
Search for more papers by this authorDr. Jaewoong Lim
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorGrace C. Thaggard
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorYuan Liu
Department of Materials Science and Engineering, University of Florida, Gainesville, FL 32611 USA
Search for more papers by this authorDr. Corey R. Martin
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorDr. Gabrielle A. Leith
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorDonald J. Toler
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorDr. An T. Ta
Department of Materials Science and Engineering, University of Florida, Gainesville, FL 32611 USA
Search for more papers by this authorDr. Nancy Birkner
Department of Materials Science and Engineering, Clemson University, Clemson, SC 29634 USA
Center for Nuclear Environmental Engineering Sciences and Radioactive Waste Management (NEESRWM), Clemson University, Clemson, SC 29634 USA
Search for more papers by this authorDr. Ingrid Lehman-Andino
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorDr. Alejandra Hernandez-Jimenez
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorDr. Gregory Morrison
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorDr. Jake W. Amoroso
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorProf. Dr. Hans-Conrad zur Loye
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorDr. Dave P. DiPrete
Savannah River National Laboratory, Aiken, SC 29808 USA
Search for more papers by this authorDr. Mark D. Smith
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorProf. Dr. Kyle S. Brinkman
Department of Materials Science and Engineering, Clemson University, Clemson, SC 29634 USA
Center for Nuclear Environmental Engineering Sciences and Radioactive Waste Management (NEESRWM), Clemson University, Clemson, SC 29634 USA
Search for more papers by this authorProf. Dr. Simon R. Phillpot
Department of Materials Science and Engineering, University of Florida, Gainesville, FL 32611 USA
Search for more papers by this authorCorresponding Author
Prof. Dr. Natalia B. Shustova
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC 29208 USA
Search for more papers by this authorGraphical Abstract
Like baking cookies to personal taste, preparation of a library of heterometallic actinide-MOFs allows for tailoring of the “flavor” of material properties. Mixing the radionuclide ingredients in proper ratios reveals structure–property relationships and unique design principles for new classes of actinide-based materials. In addition, the prepared frameworks provide a recipe for novel, pre-designed transuranic MOFs.
Abstract
A novel series of heterometallic f-block-frameworks including the first examples of transuranic heterometallic 238U/239Pu-metal–organic frameworks (MOFs) and a novel monometallic 239Pu-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.
Conflict of interest
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available in the supplementary material of this article.
Supporting Information
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| anie202216349-sup-0001-SI_Pu-Me2BPDC-12.cif156.3 KB | Supporting Information |
| anie202216349-sup-0001-SI_Th-BPyDC-12.cif5.8 MB | Supporting Information |
| anie202216349-sup-0001-SI_U-Me2BPDC-8.cif3.3 MB | Supporting Information |
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