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Equatorial coordination optimization for enhanced axiality of mononuclear Dy(iii) single-molecule magnets
Ke-Xin Yu1, You-Song Ding, Yuan-Qi Zhai
1Frontier Institute of Science and Technology (FIST), School of Science, Research Institute of Xi'an Jiaotong University (Zhejiang), State Key Laboratory of Mechanical Behavior for Materials, MOE Key Laboratory for Nonequilibrium Synthesis of Condensed Matter, Xi'an Key Laboratory of Sustainable Energy and Materials Chemistry, Xi'an Jiaotong University, 99 Yanxiang Road, Xi'an, Shaanxi 710054, P. R. China. hantian0123@xjtu.edu.cn zheng.yanzhen@xjtu.edu.cn.
Abstract:
We present a controlled synthetic route to optimize the equatorial coordination environment of three Dy(iii) borohydride complexes: Dy(BH4)3(THF)3 (1), [Dy(BH4)2(THF)5][BPh4] (2) and [Dy(BH4)2(18-C-6)][Na(THF)2(18-C-6)][BPh4]2 (3) (THF = tetrahydrofuran, BPh4- = tetraphenyl borate, 18-C-6 = 18-crown-6-ether), which have the same axial coordination environment, while different equatorial sites. Alteration of the coordination environment on the equatorial sites leads to a significant change in their magnetic properties. In the absence of the dc field, complex 1 with three THF molecules and one BH4- ligand in the equatorial plane shows no single-molecule magnet (SMM) behaviour, complex 2 having five THF molecules at equatorial sites displays small tails of out-of-phase (χ'') signals, and complex 3 containing one 18-C-6 with six O atoms in the equatorial plane exhibits χ'' signals at higher temperatures. These results show the optimization of the equatorial coordination environment of Dy(iii) mononuclear single-molecule magnets.
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