期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 27, 期 39, 页码 10012-10015出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202101239
关键词
cages; chirality; palladium; P-N ligands; radicals
资金
- SERB, India [CRG/2019/004615]
- DST [DST/SJF/CSA-03/2018-10]
- SERB [CRG/2018/000430, SB/SJF/2019-20/12, SPR/2019/001145]
This study reports a stable polyradical tetrahedral palladium(II) cage and reveals its stability mechanism and structure through experimental and theoretical calculations. The research shows that under specific conditions, the diradical state in the cage is more stable than the monoradical state, and there is a weak ferromagnetic exchange observed between adjacent radical centers in the DFT studies.
The synthesis of cages with a polyradical framework remains a challenging task. Herein is reported an enantiomeric pair of quinoid-bridged polyradical tetrahedral palladium(II) cages that are stabilized by an unusual dianionic diradical form (dhbq(..2-)). These cages have been characterized by electron paramagnetic resonance and UV-visible spectroscopy, squid magnetometry and mass spectrometry. Single-crystal-derived X-ray investigations of the iso-structural cages built on fluoranilate linkers confirm the tetrahedral structure of the obtained radical cages. Theoretical calculations showed that the diradical state of the dhbq anions is more stable than the usual monoradical state. A weak ferromagnetic exchange between adjacent radical centers was observed in DFT studies.
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