Journal
DALTON TRANSACTIONS
Volume 44, Issue 48, Pages 20867-20873Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5dt03363b
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Funding
- National Science Foundation of China [91326112, 21422704, 21561018, 11475044, 41461070]
- Science Foundation of Jiangsu Province [BK20140007]
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- Jiangsu Provincial Key Laboratory of Radiation Medicine and Protection, Young Thousand Talented Program in China
- National Basic Research Program of China [2014CB460604]
- Program for Changjiang Scholars and Innovative Research Team in University [IRT13054]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Heavy Elements Chemistry Program [DE-FG02-13ER16414]
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The solvothermal reaction of thorium nitrate and tris-(4-carboxylphenyl)phosphine oxide in DMF affords a centrosymmetric porous thorium organic framework compound [Th(TPO)(OH)(H2O)]center dot 8H(2)O (1). In contrast, the ionothermal reaction of the same reagents in the ionic liquid 1-butyl-2,3-dimethylimidazolium chloride results in the formation of a rare example of a chiral and porous thorium organic framework compound, [C9H17N2][Th(TPO)Cl-2]center dot 18H(2)O (2), which is derived solely from achiral starting materials. The geometries of the Th(IV) centers in compounds 1 and 2 are both atypical for low valent actinides, which can be best described as a ten-coordinate spherical sphenocorona and an irregular muffin, respectively. A large cavity of 17.5 angstrom (max. face to face) x 8 angstrom (min. face to face) with a BET surface area of 623 m(2) g(-1) in compound 2 is observed. The poor stability indicated by thermal gravimetric analysis and the water-resistance test for compound 2 may be due to the unique anisotropic coordination geometry for thorium. Temperature-dependent luminescence studies for both compounds indicate that the trends in the intensity vary as the Th-Th distance and the coordination environments of Th(IV) centers change.
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