TY - JOUR
T1 - Advancement of Actinide Metal-Organic Framework Chemistry via Synthesis of Pu-UiO-66
AU - Hastings, Ashley M.
AU - Ray, Debmalya
AU - Jeong, Wooseok
AU - Gagliardi, Laura
AU - Farha, Omar K.
AU - Hixon, Amy E.
N1 - Publisher Copyright:
© 2020 American Chemical Society.
PY - 2020/5/20
Y1 - 2020/5/20
N2 - We report the synthesis and characterization of the first plutonium metal-organic framework (MOF). Pu-UiO-66 expands the established UiO-66 series, which includes transition metal, lanthanide, and early actinide elements in the hexanuclear nodes. The thermal stability and porosity of Pu-UiO-66 were experimentally determined, and multifaceted computational methods were used to corroborate experimental values, examine inherent defects in the framework, decipher spectroscopic signatures, and elucidate the electronic structure. The crystallization of a plutonium chain side product provides direct evidence of the competition that occurs between modulator and linker in MOF syntheses. Ultimately, the synthesis of Pu-UiO-66 demonstrates adept control of Pu(IV) coordination under hydrolysis-prone conditions, provides an opportunity to extend trends across isostructural UiO-66 frameworks, and serves as the foundation for future plutonium MOF chemistry.
AB - We report the synthesis and characterization of the first plutonium metal-organic framework (MOF). Pu-UiO-66 expands the established UiO-66 series, which includes transition metal, lanthanide, and early actinide elements in the hexanuclear nodes. The thermal stability and porosity of Pu-UiO-66 were experimentally determined, and multifaceted computational methods were used to corroborate experimental values, examine inherent defects in the framework, decipher spectroscopic signatures, and elucidate the electronic structure. The crystallization of a plutonium chain side product provides direct evidence of the competition that occurs between modulator and linker in MOF syntheses. Ultimately, the synthesis of Pu-UiO-66 demonstrates adept control of Pu(IV) coordination under hydrolysis-prone conditions, provides an opportunity to extend trends across isostructural UiO-66 frameworks, and serves as the foundation for future plutonium MOF chemistry.
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U2 - 10.1021/jacs.0c01895
DO - 10.1021/jacs.0c01895
M3 - Article
C2 - 32337982
AN - SCOPUS:85087396560
SN - 0002-7863
VL - 142
SP - 9363
EP - 9371
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 20
ER -