期刊
CHEMICAL SCIENCE
卷 8, 期 3, 页码 2073-2080出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6sc04465d
关键词
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资金
- European Research Council for the Consolidator [646740]
- EPSRC [EP/M022064/1]
- Engineering and Physical Sciences Research Council [EP/M022064/1] Funding Source: researchfish
- EPSRC [EP/M022064/1] Funding Source: UKRI
- European Research Council (ERC) [646740] Funding Source: European Research Council (ERC)
Single-molecule magnets (SMMs) are coordination compounds that exhibit magnetic bistability below a characteristic blocking temperature. Research in this field continues to evolve from its fundamental foundations towards applications of SMMs in information storage and spintronic devices. Synthetic chemistry plays a crucial role in targeting the properties that could ultimately produce SMMs with technological potential. The ligands in SMMs are invariably based on non-metals; we now report a series of dysprosium SMMs (in addition to their magnetically dilute analogues embedded in yttrium matrices) that contain ligands with the metalloid element antimony as the donor atom, i.e. [(eta(5)-Cp'Dy-2){mu-Sb(H)Mes}](3) (1-Dy) and [(eta(5)-Cp'Dy-2) (3){mu-(SbMes)(3)Sb}] (2-Dy), which contain the stibinide ligand [Mes(H)Sb](-) and the unusual Zintl-like ligand [Sb(4)Mes(3)](3-), respectively (Cp' = methylcyclo pentadienyl; Mes = mesityl). The zero-field anisotropy barriers in 1-Dy and 2-Dy are U-eff = 345 cm(-1) and 270 cm(-1), respectively. Stabilization of the antimony-ligated SMMs is contingent upon careful control of reaction time and temperature. With longer reaction times and higher temperatures, the stibine pro-ligands are catalytically dehydrocoupled by the rare-earth precursor complexes. NMR spectroscopic studies of the yttrium-catalysed dehydrocoupling reactions reveal that 1-Y and 2-Y are formed during the catalytic cycle. By implication, 1-Dy and 2-Dy should also be catalytic intermediates, hence the nature of these complexes as SMMs in the solid-state and as catalysts in solution introduces a strategy whereby new molecular magnets can be identified by intercepting species formed during catalytic reactions.
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