Structural Features of Zirconium-Based Metal–Organic Frameworks Affecting Radiolytic Stability

Hanna, Sylvia L.; Rademacher, David X.; Hanson, Donald J.; Islamoglu, Timur; Olszewski, Alyssa K.; Nenoff, Tina M.; Farha, Omar K.

doi:10.1021/acs.iecr.9b06820

Structural Features of Zirconium-Based Metal–Organic Frameworks Affecting Radiolytic Stability

Journal Article · Wed Apr 01 00:00:00 EDT 2020 · Industrial and Engineering Chemistry Research

DOI:https://doi.org/10.1021/acs.iecr.9b06820· OSTI ID:1615770

^[1]; Rademacher, David X. ^[2]; Hanson, Donald J. ^[2]; ^[3]; Olszewski, Alyssa K. ^[3]; ^[2]; ^[3]

Northwestern Univ., Evanston, IL (United States); University of Notre Dame
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Northwestern Univ., Evanston, IL (United States)

Metal–organic frameworks (MOFs) NU-1000 and UiO-66 are herein exposed to two different gamma irradiation doses and dose rates and analyzed to determine the structural features that affect their stability in these environments. MOFs have shown promise for the capture and sensing of off-gases at civilian nuclear energy reprocessing sites, nuclear waste repositories, and nuclear accident locations. However, little is understood about the structural features of MOFs that contribute to their stability levels under the ionizing radiation conditions present at such sites. This study is the first of its kind to explore the structural features of MOFs that contribute to their radiolytic stability. Both NU-1000 and UiO-66 are MOFs that contain Zr metal-centers with the same metal absorption cross section. However, the two MOFs exhibit different linker connectivities, linker aromaticities, node densities, node connectivities, and interligand separations. In this study, NU-1000 and UiO-66 were exposed to high (423.3 Gy/min, 23 min, and 37 s) and low (0.78 Gy/min, 4320 min) dose rates of ⁶⁰Co gamma irradiation. NU-1000 displayed insignificant radiation damage under both dose rates due to its high linker connectivity, low node density, and low node connectivity. However, low radiation dose rates caused considerable damage to UiO-66, a framework with lower aromaticity and smaller interligand separation. Finally, results suggest that chronic, low-radiation environments are more detrimental to Zr MOF stability than acute, high-radiation conditions.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003763; SC0012577; NA0003525

OSTI ID:: 1615770

Alternate ID(s):: OSTI ID: 1618072

Journal Information:: Industrial and Engineering Chemistry Research, Journal Name: Industrial and Engineering Chemistry Research Journal Issue: 16 Vol. 59; ISSN 0888-5885

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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