Expanding the Transuranic Metal–Organic Framework Portfolio: The Optical Properties of Americium(III) MOF-76

Arteaga, Ana L.; Nicholas, Aaron D.; Sinnwell, Michael A.; McNamara, Bruce K.; Buck, Edgar C.; Surbella, Robert G.

doi:10.1021/acs.inorgchem.3c02742

Title: Expanding the Transuranic Metal–Organic Framework Portfolio: The Optical Properties of Americium(III) MOF-76

Journal Article · 30 November 2023 · Inorganic Chemistry

DOI: https://doi.org/10.1021/acs.inorgchem.3c02742 · OSTI ID:2340837

Arteaga, Ana L. ^[1];

^[1];

^[1]; McNamara, Bruce K. ^[1];

^[1];

^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Reported here is the synthesis, crystal structure, and solid-state characterization of a new americium containing metal–organic framework (MOF), [Am(C₉H₃O₆)(H₂O)], MOF-76(Am). This material is constructed from Am³⁺ metal centers and 1,3,5-tricarboxylic acid (BTC) ligands, forming a porous three-dimensional framework that is isostructural with several known trivalent lanthanide (Ln) analogs (e.g., Ce, Nd, and Sm–Lu). The Am³⁺ ions have seven coordinates and assume a distorted, capped trigonal prismatic geometry with C1 symmetry. The Am³⁺–O bonds were studied via infrared spectroscopy and compared to several MOF-76(Ln) analogs, where Ln = Nd³⁺, Eu³⁺, Tb³⁺, and Ho³⁺. The results show that the strength of the ligand carboxylate stretching and bending modes increase with Nd³⁺ < Eu³⁺ < Am³⁺ < Tb³⁺ < Ho³⁺, suggesting the metal–oxygen bonds are predominantly ionic. Optical absorbance spectroscopy measurements reveal strong f–f transitions; some exhibit pronounced crystal field splitting. The photoluminescence spectrum contains weak Am³⁺-based emission that is achieved through direct and indirect metal center excitation. The weak emissive behavior is somewhat surprising given that ligand-to-metal resonance energy transfer is efficient in the isoelectronic Eu³⁺ (4f⁶) and related Tb³⁺ (4f⁸) analogs. The optical properties were explored further within a series of heterometallic MOF-76(Tb_1–xAm_x) (x = 0.8, 0.2, and 0.1) samples, and the results reveal enhanced Am³⁺ photoluminescence.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2340837

Report Number(s):: PNNL-SA--186142

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 51 Vol. 62; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Expanding the Transuranic Metal–Organic Framework Portfolio: The Optical Properties of Americium(III) MOF-76

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