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Cyanido-Bridged Clusters with Remote N-Oxide Groups for Branched Multimetallic Systems

机译：Cyanido-Bridged簇具有用于分支多金属系统的远程N-氧化物组

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摘要

The combination of [W-V(CN)(8)](3-) anions with 3d metal cations M-II in MeOH leads to the formation of pentadecanuclear spherical cyanido-bridged clusters {M[M(solv)(3)](8)[M'(CN)(8)](6)}, M9M'(6). By decorating their surface with organic ligands or/and by installation of different ions in their coordination skeleton, one could tune high spin in the ground state, slow relaxation of magnetization, or structural/spin phase transition. In this work we present the extended molecular high spin (S-GS = 15/2, g(eff) = 3.4) clusters or chains of clusters {Co9W6(N,O-L)(x)} (N,O-L - pyrazine mono-N-oxide, pzmo; 4,4-bipyridine mono-N-oxide - 4,4'-bpmo) equipped with the structurally ordered remote (2-2.5 nm) N-oxide functions, as a result of deliberate combination of solvated Co9W6 supercomplexes with asymmetric N,O-donor linkers L. The systematic occurrence of such motifs in the series 1-3 is a result of preference for the Co-N-L coordination over the Co-O-L coordination, controlled also by strongly competing supramolecular interactions including simple hydrogen bonding {LNO center dot center dot center dot H-donor} as well as cooperative pi-costacked hydrogen bonding in double cyclic synthons {Co-O-H-MeOH center dot center dot center dot O-NbpmoN-}(2). The observed coordination backbones are discussed in terms of the potential to bind the specific external molecular units and create the new type of branched molecular organization. The magnetic properties are confronted with structural differences along 1-3, considering coordination polyhedra, Co-N bond lengths, Co-N-C angles, and hydrogen bonds. The diversity of slow magnetic relaxation images for the known Co9W6 based phases are discussed in terms of local deformation of Co coordination polyhedra and global deformation of cyanide bridged backbones.
机译：MeOH中3D金属阳离子M-II的[WV（CN）（8）（8）个]（3-）阴离子的组合导致戊天竺葵球形氰基桥簇的形成{M [M（SOLV）（3）]（8 ）[m'（cn）（8）]（6）}，m9m'（6）。通过用有机配体或通过在其协调骨架中安装不同的离子来装饰它们的表面，可以在地状态下调整高旋转，磁化缓慢放松，或结构/旋转相转变。在这项工作中，我们呈现扩展的分子高旋转（S-GS = 15/2，G（EFF）= 3.4）簇簇或链簇{CO 9W6（N，OL）（x）}（n，ol - 吡嗪单 - N-氧化物，PZMO; 4,4-硼吡啶单-N-氧化物 - 4,4'-BPMO），其配备有结构有序的偏远（2-2.5nm）N-氧化物功能，其结果是溶解的CO9W6的腐败组合具有不对称N，O-供体接头L的超复杂性。第1-3系列中这种基序的系统发生是通过强烈竞争的超分子相互作用而对CO-OL协调进行CO-NL协调的优选。氢键{LNO中心点中心点中心点H·捐助}以及双循环合成器中的合作PI-Costached氢键{Co-Oh-Meoh中心DOT中心DOT中心DOT O-NBPMON - }（2）。观察到的配位骨干在结合特定外部分子单元的潜力方面讨论并产生新型分子组织。考虑到协调多面体，CO-N键长，CO-N-C角度和氢键，磁性特性面对结构差异。在CO协调多面体的局部变形和氰化物桥接骨干的全局变形的局部变形方面讨论了已知的CO9W6基相的缓慢磁性弛豫图像的多样性。

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  • 来源
    《Crystal growth & design》 |2018年第8期|共11页
  • 作者

    Kobylarczyk Jedrzej; Augustyniak Klaudia; Chorazy Szymon; Nowicka Beata; Pinkowicz Dawid; Koziel Marcin; Muziol Tadeusz; Podgajny Robert;

  • 作者单位

    Jagiellonian Univ Fac Chem Gronostajowa 2 PL-30387 Krakow Poland;

    Jagiellonian Univ Fac Chem Gronostajowa 2 PL-30387 Krakow Poland;

    Jagiellonian Univ Fac Chem Gronostajowa 2 PL-30387 Krakow Poland;

    Jagiellonian Univ Fac Chem Gronostajowa 2 PL-30387 Krakow Poland;

    Jagiellonian Univ Fac Chem Gronostajowa 2 PL-30387 Krakow Poland;

    Jagiellonian Univ Fac Chem Gronostajowa 2 PL-30387 Krakow Poland;

    Nicolaus Copernicus Univ Fac Chem Jurija Gagarina 7 PL-87100 Torun Poland;

    Jagiellonian Univ Fac Chem Gronostajowa 2 PL-30387 Krakow Poland;

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  • 正文语种 eng
  • 中图分类 晶体学;
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