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.

doi:10.1002/ange.202216349

f‐ block MOFs: A Pathway to Heterometallic Transuranics

Journal Article · Mon Dec 19 00:00:00 EST 2022 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202216349· OSTI ID:1910282

^[1]; Kittikhunnatham, Preecha ^[2]; ^[1]; Thaggard, Grace C. ^[1]; ^[3]; Martin, Corey R. ^[4]; Leith, Gabrielle A. ^[1]; Toler, Donald J. ^[1]; ^[3]; Birkner, Nancy ^[5]; Lehman‐Andino, Ingrid ^[4]; Hernandez‐Jimenez, Alejandra ^[4]; Morrison, Gregory ^[1]; ^[4]; zur Loye, Hans‐Conrad ^[6]; DiPrete, Dave P. ^[4]; Smith, Mark D. ^[1]; ^[5]; ^[3]; ^[1]

Department of Chemistry and Biochemistry University of South Carolina Columbia SC 29208 USA
Department of Chemistry Chulalongkorn University Bangkok 10330 Thailand
Department of Materials Science and Engineering University of Florida Gainesville FL 32611 USA
Savannah River National Laboratory Aiken SC 29808 USA
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
Department of Chemistry and Biochemistry University of South Carolina Columbia SC 29208 USA, Savannah River National Laboratory Aiken SC 29808 USA

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.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0016574

OSTI ID:: 1910282

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 5 Vol. 135; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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