A Series of [Co(Mabiq)Cl2-n] (n = 0, 1, 2) Compounds and Evidence for the Elusive Bimetallic Form.

A Series of [Co(Mabiq)Cl2-n] (n = 0, 1, 2) Compounds and Evidence for the Elusive Bimetallic Form.
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一系列 [Co(Mabiq)Cl2-n] (n = 0, 1, 2) 化合物和难以捉摸的双金属形式的证据。

DOI：
10.1021/acs.inorgchem.5b00636
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发表时间：
2015
期刊：
Inorganic chemistry
影响因子：
4.6
通讯作者：
Corinna R. Hess
Corinna R. Hess
中科院分区：
化学2区
文献类型：
--
作者：
E. Puttock;P. Banerjee;Manuel Kaspar;Liam Drennen;D. Yufit;E. Bill;Stephen Sproules;Corinna R. Hess

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合成了一系列具有氧化还原活性的大环双喹唑啉配体Mabiq [2-4：6-8-双（3，3，4，4-四甲基二氢吡咯）-10-15-（2，2 '-双喹唑啉）-[15]-1，3，5，8，10，14-六烯-1，3，7，9，11，14-N6]配位的钴化合物，并对其结构进行了表征.该系列包括单金属化合物Co（Mabiq）Cl 2（1）、Co（Mabiq）Cl（2）和Co（Mabiq）（4），其形式金属氧化态为3+ → 1+。此外，还获得了双核钴化合物Co2（Mabiq）Cl 3（3），首次证明了Mabiq配体能够配位两个金属离子。顺磁性2和3的电子结构进行了研究，通过电子顺磁共振谱和磁化率的研究。位于2和3的N4-大环腔中的Co（II）离子采用低自旋S =（1）/2构型。3中的bypirimidine官能团另外在四面体环境中配位高自旋S =（3）/2钴离子。3中的两个金属离子通过磁力测定法弱耦合。正方形平面的低价4提供了有限数量的结构特征为N4-大环Co（I）化合物的实例之一。光谱和密度泛函理论计算数据表明，Co（II）（Mabiq（·））描述可能是该化合物的Co（I）形式主义的合理替代。
The synthesis and characterization of a series of cobalt compounds, coordinated by the redox-active macrocyclic biquinazoline ligand, Mabiq [2-4:6-8-bis(3,3,4,4-tetramethyldihydropyrrolo)-10-15-(2,2'-biquinazolino)-[15]-1,3,5,8,10,14-hexaene-1,3,7,9,11,14-N6], is presented. The series includes the monometallic Co(Mabiq)Cl2 (1), Co(Mabiq)Cl (2), and Co(Mabiq) (4), with formal metal oxidation states of 3+ → 1+. A binuclear cobaltous compound, Co2(Mabiq)Cl3 (3), also was obtained, providing the first evidence for the ability of the Mabiq ligand to coordinate two metal ions. The electronic structures of the paramagnetic 2 and 3 were examined by electron paramagnetic resonance spectroscopy and magnetic susceptibility studies. The Co(II) ion that resides in the N4-macrocylic cavity of 2 and 3 adopts a low-spin S = (1)/2 configuration. The bypirimidine functionality in 3 additionally coordinates a high-spin S = (3)/2 cobaltous ion in a tetrahedral environment. The two metal ions in 3 are weakly coupled by magnetometry. The square-planar, low-valent 4 offers one of a limited number of examples of structurally characterized N4-macrocyclic Co(I) compounds. Spectroscopic and density functional theory computational data suggest that a Co(II)(Mabiq(•)) description may be a reasonable alternative to the Co(I) formalism for this compound.