Influence of Linker Identity on the Photochemistry of Uranyl-Organic Frameworks

Knapp, Julia G.; Livshits, Maksim Y.; Gilhula, J. Connor; Hanna, Sylvia L.; Piedmonte, Ida D.; Rice, Natalie T.; Wang, Xingjie; Stein, Benjamin W.; Kozimor, Stosh A.; Farha, Omar K.

doi:10.1021/acsami.3c06897

Influence of Linker Identity on the Photochemistry of Uranyl-Organic Frameworks

Journal Article · Wed Sep 06 00:00:00 EDT 2023 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.3c06897· OSTI ID:2007796

^[1]; ^[2]; Gilhula, J. Connor ^[2]; ^[3]; Piedmonte, Ida D. ^[2]; Rice, Natalie T. ^[2]; ^[3]; ^[2]; ^[2]; ^[3]

Northwestern University, Evanston, IL (United States); University of Notre Dame
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Northwestern University, Evanston, IL (United States)

While uranyl-based metal–organic frameworks (MOFs) boast impressive photocatalytic abilities, significant questions remain regarding their excitation pathways and methods to fine-tune their performance due to the lack of information regarding heterogeneous uranyl catalysis. Herein, we investigated how linker identity and photoexcitation impact uranyl photocatalysis when the uranyl coordination environment remains constant. Toward this end, we prepared three uranyl-based MOFs (NU-1301, NU-1307, and ZnTCPP-U2) and then examined the structural and photochemical properties of each through X-ray diffraction, X-ray absorption, and photoluminescence. We then correlated our observations to the photocatalytic performance for fluorination of cyclooctane. The excitation profile from NU-1301 and NU-1307 exhibited spin-forbidden linker transitions and uranyl vibronic progressions, with uranyl excitation and emission being most dominant in NU-1301. Consequently, NU-1301 was a more active photocatalyst than NU-1307. In contrast, the excitation profile from ZnTCPP-U2 contained transitions associated with the porphyrin linker exclusively. Photocatalytic activity from ZnTCPP-U2 significantly underperformed in comparison to that of the other two MOFs. Furthermore, these data suggest that linkers’ photophysical properties can be used to predict the photocatalytic behavior of uranyl-containing MOFs.

View Accepted Manuscript (DOE)

Research Organization:: University of Notre Dame, IN (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515; NA0003763

OSTI ID:: 2007796

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 37 Vol. 15; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Influence of Linker Identity on the Photochemistry of Uranyl-Organic Frameworks

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