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Title: Stabilization of an Unprecedented Hexanuclear Secondary Building Unit in a Thorium-Based Metal–Organic Framework

Abstract

The crystal structures of thorium clusters are important for understanding the formation and transformation mechanisms of actinide species in solution, which can in turns benefit nuclear waste processing and management. However, stabilizing thorium clusters in aqueous solution is quite challenging because of their fast olation and oxolation reactions. Here, we report a thorium-based meta-organic framework, NU-905, with the formula [Th 63-O) 2(HCOO) 4(H 2O) 6] [TCPP = tetrakis(4-carboxyphenyl)porphyrin], synthesized by a solvothermal reaction in N,N-dimethylformamide and water at 120 °C. NU-905 contains a hexanuclear secondary building unit (SBU), [Th 63-O) 2(HCOO) 4(H 2O) 6], which has never been reported previously. The SBUs are capped and bridged by the tetratopic linker TCPP to form a three-dimensional network with scu topology. The activated NU-905 exhibits permanent porosity and shows high catalytic activity for the selective photooxidation of a mustard gas simulant.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States); South China Univ. of Technology (SCUT), Guangzhou (China). School of Chemistry and Chemical Engineering
Publication Date:
Research Org.:
Univ. of Notre Dame, Notre Dame, IN (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1497854
Grant/Contract Number:  
NA0003763
Resource Type:
Accepted Manuscript
Journal Name:
Inorganic Chemistry
Additional Journal Information:
Journal Volume: 58; Journal Issue: 6; Journal ID: ISSN 0020-1669
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Li, Peng, Goswami, Subhadip, Otake, Ken-ichi, Wang, Xingjie, Chen, Zhijie, Hanna, Sylvia L., and Farha, Omar K.. Stabilization of an Unprecedented Hexanuclear Secondary Building Unit in a Thorium-Based Metal–Organic Framework. United States: N. p., 2019. Web. doi:10.1021/acs.inorgchem.8b03511.
Li, Peng, Goswami, Subhadip, Otake, Ken-ichi, Wang, Xingjie, Chen, Zhijie, Hanna, Sylvia L., & Farha, Omar K.. Stabilization of an Unprecedented Hexanuclear Secondary Building Unit in a Thorium-Based Metal–Organic Framework. United States. doi:10.1021/acs.inorgchem.8b03511.
Li, Peng, Goswami, Subhadip, Otake, Ken-ichi, Wang, Xingjie, Chen, Zhijie, Hanna, Sylvia L., and Farha, Omar K.. Mon . "Stabilization of an Unprecedented Hexanuclear Secondary Building Unit in a Thorium-Based Metal–Organic Framework". United States. doi:10.1021/acs.inorgchem.8b03511.
@article{osti_1497854,
title = {Stabilization of an Unprecedented Hexanuclear Secondary Building Unit in a Thorium-Based Metal–Organic Framework},
author = {Li, Peng and Goswami, Subhadip and Otake, Ken-ichi and Wang, Xingjie and Chen, Zhijie and Hanna, Sylvia L. and Farha, Omar K.},
abstractNote = {The crystal structures of thorium clusters are important for understanding the formation and transformation mechanisms of actinide species in solution, which can in turns benefit nuclear waste processing and management. However, stabilizing thorium clusters in aqueous solution is quite challenging because of their fast olation and oxolation reactions. Here, we report a thorium-based meta-organic framework, NU-905, with the formula [Th6(μ3-O)2(HCOO)4(H2O)6] [TCPP = tetrakis(4-carboxyphenyl)porphyrin], synthesized by a solvothermal reaction in N,N-dimethylformamide and water at 120 °C. NU-905 contains a hexanuclear secondary building unit (SBU), [Th6(μ3-O)2(HCOO)4(H2O)6], which has never been reported previously. The SBUs are capped and bridged by the tetratopic linker TCPP to form a three-dimensional network with scu topology. The activated NU-905 exhibits permanent porosity and shows high catalytic activity for the selective photooxidation of a mustard gas simulant.},
doi = {10.1021/acs.inorgchem.8b03511},
journal = {Inorganic Chemistry},
number = 6,
volume = 58,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
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This content will become publicly available on February 25, 2020
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