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High Uptake of ReO 4 − and CO 2 Conversion by a Radiation‐Resistant Thorium–Nickle [Th 48 Ni 6 ] Nanocage‐Based Metal–Organic Framework
Author(s) -
Xu Hang,
Cao ChunShuai,
Hu HanShi,
Wang ShiBin,
Liu JinCheng,
Cheng Peng,
Kaltsoyannis Nikolas,
Li Jun,
Zhao Bin
Publication year - 2019
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201901786
Subject(s) - nanocages , thorium , catalysis , metal , aromaticity , transition metal , chemical stability , nuclear chemistry , chemistry , materials science , crystallography , organic chemistry , molecule , metallurgy , uranium
Assembled from [Th 48 Ni 6 ] nanocages, the first transition‐metal (TM)‐thorium metal–organic framework (MOF, 1 ) has been synthesized and structurally characterized. 1 exhibits high solvent and acid/base stability, and resistance to 400 kGy β irradiation. Notably, 1 captures ReO 4 − (an analogue of radioactive 99 TcO 4 − , a key species in nuclear wastes) with a maximum capacity of 807 mg g −1 , falling among the largest values known to date. Furthermore, 1 can enrich methylene blue (MB) and can also serve as an effective and recyclable catalyst for CO 2 fixation with epoxides; there is no significant loss of catalytic activity after 10 cycles. Theoretical studies with nucleus‐independent chemical shifts and natural bond orbital analysis reveal that the [Th 6 O 8 ] clusters in 1 have a unique stable electronic structure with (d–p)π aromaticity, partially rationalising 1 ′s stability.