Role of Metal Selection in the Radiation Stability of Isostructural M-UiO-66 Metal–Organic Frameworks

Hastings, Ashley M.; Fairley, Melissa; Wasson, Megan C.; Campisi, Dario; Sarkar, Arup; Emory, Zoë C.; Brunson, Kieran; Fast, Dylan B.; Islamoglu, Timur; Nyman, May; Burns, Peter C.; Gagliardi, Laura; Farha, Omar K.; Hixon, Amy E.; LaVerne, Jay A.

doi:10.1021/acs.chemmater.2c02170

Title: Role of Metal Selection in the Radiation Stability of Isostructural M-UiO-66 Metal–Organic Frameworks

Journal Article · Fri Sep 09 00:00:00 EDT 2022 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.2c02170· OSTI ID:1886847

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Univ. of Notre Dame, IN (United States)
Univ. of Notre Dame, IN (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Northwestern Univ., Evanston, IL (United States)
Univ. of Chicago, IL (United States)
Oregon State Univ., Corvallis, OR (United States)

Robust and versatile metal–organic frameworks (MOFs) have emerged as sophisticated scaffolds to meet the critical needs of the nuclear community, but their performance depends on their underexplored structural integrities in high- radiation fields. The contributions of selected metal nodes in the radiation stability of MOFs within the isostructural M-UiO-66 series (where M = Zr, Ce, Hf, Th, and Pu; Zr-UiO-66 experiments were executed in a previous work) have been determined. Ce-, Hf-, and Th-UiO-66 MOF samples were irradiated via gamma and He-ion methodologies to obtain doses up to 3 MGy and 85 MGy, respectively, the latter strikingly higher than that obtained in most other studies. Appreciable self-irradiation constituted the total absorbed doses, up to 31 MGy of the gamma-irradiated Pu-UiO-66 samples. Structural degradation was ascertained by powder X-ray diffraction, X-ray total scattering, vibrational spectroscopy, and, where possible, N₂ physisorption isotherms. Diffuse reflectance infrared Fourier transform spectroscopy provided atomic-level mechanistic insights to reveal that the node-linker connection was most susceptible to radiation damage. Density functional theory calculations were performed on cluster models to evaluate the binding energy of the linkers to each metal node. Here, while the isostructures disclosed the same breakdown signatures, distinct radiation sensitivity as a function of metal selection was evident and followed the trend Hf-UiO-66 ~ Zr-UiO-66 > Th-UiO-66 > Pu-UiO-66 > Ce-UiO-66. We anticipate that these endeavors will contribute to the rational design of radiation-resistant materials for targeted applications.

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

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003763

OSTI ID:: 1886847

Journal Information:: Chemistry of Materials, Vol. 34, Issue 18; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Role of Metal Selection in the Radiation Stability of Isostructural M-UiO-66 Metal–Organic Frameworks

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