期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 26, 期 39, 页码 8621-8630出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202001365
关键词
biradical; crystal engineering; magnetic anisotropy; NMR; redox
资金
- Japan Society for the Promotion of Science (JSPS) KAKENHI [JP14J02656, JP20225003, JP15K05467, JP24750119, 18K14242, 19K05401]
- Tohoku University Molecule & Material Synthesis Platform in Nanotechnology Platform Project, CREST, JST [JPMJCR12L3]
- Beilstein-Institut zur Forderung der Chemischen Wissenschaften
- German-Japanese University Consortium (HeKKSaGOn)
- state of Baden-Wurttemberg through bwHPC
- German Research Foundation (DFG) [INST 40/467-1 FUGG]
- European Union [ERC StG 2012-306826]
- Networking Research Center on Bioengineering, Biomaterials, and Nanomedicine (CIBER-BBN)
- Spanish Ministry of Economy and Competitiveness [FANCY CTQ2016-80030-R, MOTHER MAT2016-80826-R]
- Generalitat de Catalunya [2017SGR918]
- 111 Project from China [B18030]
- National University of Singapore [R-143-000-A80-114, R-143-000-A65-133]
- Spanish Ministry of Economy and Competitiveness (Severo Ochoa Programme for Centers of Excellence in RD) [SEV-2015-0496]
Presented here is a comprehensive study of highly oxidized multiple-decker complexes composed of Tb(III)and Cd(II)ions and two to five phthalocyaninato ligands, which are stabilized by electron-donatingn-butoxy groups. From X-ray structural analyses, all the complexes become axially compressed upon ligand oxidation, resulting in bowl-shaped distortions of the ligands. In addition, unusual coexistence of square antiprism and square prism geometries around metal ions was observed in +4echarged species. From paramagnetic(1)H NMR studies on the resulting series of triple, quadruple and quintuple-decker complexes, ligand oxidation leads to a decrease in the magnetic anisotropy, as predicted from theoretical calculations. Unusual paramagnetic shifts were observed in the spectra of the +2echarged quadruple and quintuple-decker complexes, indicating that those two species are actually unexpected triplet biradicals. Magnetic measurements revealed that the series of complexes show single-molecule magnet properties, which are controlled by the multi-step redox induced structural changes.
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