Unprecedented Radiation Resistant Thorium-Binaphthol Metal-Organic Framework

Sara E. Gilson; Melissa Fairley; Patrick Julien; Allen G. Oliver; Sylvia L. Hanna; Grace Arntz; Omar K. Farha; Jay A. Laverne; Peter C. Burns

doi:10.1021/jacs.0c05272

Unprecedented Radiation Resistant Thorium-Binaphthol Metal-Organic Framework

Sara E. Gilson, Melissa Fairley, Patrick Julien, Allen G. Oliver, Sylvia L. Hanna, Grace Arntz, Omar K. Farha, Jay A. Laverne, Peter C. Burns

Research output: Contribution to journal › Article › peer-review

49 Scopus citations

Abstract

A thorium-organic framework (TOF-16) containing hexameric secondary building units connected by functionalized binaphthol linkers was synthesized, characterized, and irradiated to probe its radiation resistance. Radiation stability was examined using γ-rays and 5 MeV He2+ ions to simulate α particles. γ-irradiation of TOF-16 to an unprecedented 4 MGy dose resulted in no apparent bulk structural damage visible by X-ray diffraction. To further probe radiation stability, we conducted the first He2+ ion irradiation study of a metal-organic framework (MOF). Diffraction data indicate onset of crystallinity loss upon approximately 15 MGy of irradiation and total loss of crystallinity upon exposure to approximately 25 MGy of He2+ ion irradiation. The high radiation resistance observed suggests MOFs can withstand radiation exposure at doses found in nuclear waste streams and highlights the need for a systematic approach to understand and eventually design frameworks with exceptional radiation resistance.

Original language	English
Pages (from-to)	13299-13304
Number of pages	6
Journal	Journal of the American Chemical Society
Volume	142
Issue number	31
DOIs	https://doi.org/10.1021/jacs.0c05272
State	Published - Aug 5 2020
Externally published	Yes

Funding

This work was supported by the National Nuclear Security Administration, Department of Energy, under Award Number DE-NA0003763. The Materials Characterization Facility of the Center for Sustainable Energy at Notre Dame provided spectroscopic and diffraction instrumentation. The authors thank Professor Michael Wiescher for making available the facilities of the Notre Dame Nuclear Structure Laboratory, which is supported by the U.S. National Science Foundation through Grant Number Phys-0758100, and Professor Ian Carmichael for making available the facilities of the Notre Dame Radiation Laboratory, which is supported by DOE BES Grant Number DE-FC02-04ER15533. This contribution is NDRL-5285 from the Notre Dame Radiation Laboratory. S.E.G. would like to thank Jennifer Szymanowski for insightful scientific conversations.

Funders	Funder number
Notre Dame Nuclear Structure Laboratory
National Science Foundation	Phys-0758100
U.S. Department of Energy	DE-NA0003763
Basic Energy Sciences	DE-FC02-04ER15533
National Nuclear Security Administration

Access to Document

10.1021/jacs.0c05272

Cite this

@article{8ba75d234fb74f1390ccfa238ae1a2f3,

title = "Unprecedented Radiation Resistant Thorium-Binaphthol Metal-Organic Framework",

abstract = "A thorium-organic framework (TOF-16) containing hexameric secondary building units connected by functionalized binaphthol linkers was synthesized, characterized, and irradiated to probe its radiation resistance. Radiation stability was examined using γ-rays and 5 MeV He2+ ions to simulate α particles. γ-irradiation of TOF-16 to an unprecedented 4 MGy dose resulted in no apparent bulk structural damage visible by X-ray diffraction. To further probe radiation stability, we conducted the first He2+ ion irradiation study of a metal-organic framework (MOF). Diffraction data indicate onset of crystallinity loss upon approximately 15 MGy of irradiation and total loss of crystallinity upon exposure to approximately 25 MGy of He2+ ion irradiation. The high radiation resistance observed suggests MOFs can withstand radiation exposure at doses found in nuclear waste streams and highlights the need for a systematic approach to understand and eventually design frameworks with exceptional radiation resistance.",

author = "Gilson, {Sara E.} and Melissa Fairley and Patrick Julien and Oliver, {Allen G.} and Hanna, {Sylvia L.} and Grace Arntz and Farha, {Omar K.} and Laverne, {Jay A.} and Burns, {Peter C.}",

note = "Publisher Copyright: Copyright {\textcopyright} 2020 American Chemical Society.",

year = "2020",

month = aug,

day = "5",

doi = "10.1021/jacs.0c05272",

language = "English",

volume = "142",

pages = "13299--13304",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

number = "31",

}

TY - JOUR

T1 - Unprecedented Radiation Resistant Thorium-Binaphthol Metal-Organic Framework

AU - Gilson, Sara E.

AU - Fairley, Melissa

AU - Julien, Patrick

AU - Oliver, Allen G.

AU - Hanna, Sylvia L.

AU - Arntz, Grace

AU - Farha, Omar K.

AU - Laverne, Jay A.

AU - Burns, Peter C.

PY - 2020/8/5

Y1 - 2020/8/5

N2 - A thorium-organic framework (TOF-16) containing hexameric secondary building units connected by functionalized binaphthol linkers was synthesized, characterized, and irradiated to probe its radiation resistance. Radiation stability was examined using γ-rays and 5 MeV He2+ ions to simulate α particles. γ-irradiation of TOF-16 to an unprecedented 4 MGy dose resulted in no apparent bulk structural damage visible by X-ray diffraction. To further probe radiation stability, we conducted the first He2+ ion irradiation study of a metal-organic framework (MOF). Diffraction data indicate onset of crystallinity loss upon approximately 15 MGy of irradiation and total loss of crystallinity upon exposure to approximately 25 MGy of He2+ ion irradiation. The high radiation resistance observed suggests MOFs can withstand radiation exposure at doses found in nuclear waste streams and highlights the need for a systematic approach to understand and eventually design frameworks with exceptional radiation resistance.

AB - A thorium-organic framework (TOF-16) containing hexameric secondary building units connected by functionalized binaphthol linkers was synthesized, characterized, and irradiated to probe its radiation resistance. Radiation stability was examined using γ-rays and 5 MeV He2+ ions to simulate α particles. γ-irradiation of TOF-16 to an unprecedented 4 MGy dose resulted in no apparent bulk structural damage visible by X-ray diffraction. To further probe radiation stability, we conducted the first He2+ ion irradiation study of a metal-organic framework (MOF). Diffraction data indicate onset of crystallinity loss upon approximately 15 MGy of irradiation and total loss of crystallinity upon exposure to approximately 25 MGy of He2+ ion irradiation. The high radiation resistance observed suggests MOFs can withstand radiation exposure at doses found in nuclear waste streams and highlights the need for a systematic approach to understand and eventually design frameworks with exceptional radiation resistance.

UR - http://www.scopus.com/inward/record.url?scp=85089611216&partnerID=8YFLogxK

U2 - 10.1021/jacs.0c05272

DO - 10.1021/jacs.0c05272

M3 - Article

C2 - 32678589

AN - SCOPUS:85089611216

SN - 0002-7863

VL - 142

SP - 13299

EP - 13304

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 31

ER -

Unprecedented Radiation Resistant Thorium-Binaphthol Metal-Organic Framework

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this