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首页> 外文期刊>Bulletin of the Chemical Society of Japan >14 Step-15 Electron Reversible Redox Behavior of Tetrameric Oligomer of Oxo-Bridged Triruthenium Cluster
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14 Step-15 Electron Reversible Redox Behavior of Tetrameric Oligomer of Oxo-Bridged Triruthenium Cluster

机译：14步15氧桥合三钌簇的四聚体低聚物的电子可逆氧化还原行为

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摘要

Pyrazine-bridged trimeric and tetrameric oligomers of triruthenium clusters,[{Ru_3O(CH_3CO_2)_6((CO)(py)}-(mu-pz)-{Ru_3O(CH_3CO_2)_6(CO)}-(mu-pz)-{Ru_3O(CH_3CO_2)_6(py)_2}]~+ (1) and [{Ru_3O(CH_3CO_2)_6(CO)(py)}-(mu-pz)-{Ru_3O-(CH_3CO_2)_6(CO)}-(mu-pz)-{Ru_3O(CH_3CO_2)_6(Py))-(mu-pz)-{Ru_3O(CH_3CO_2)_6(dmap)_2}]~(2+) (2),were prepared (pz=pyr-azine,py=pyridine,dmap=4-dimethylaminopyridine).Trimer 1 and tetramer 2 show closely spaced 11 step-12 electron and 14 step-15 electron reversible redox waves,respectively,in their cyclic voltammograms in CH_3CN.These compounds were designed specifically to incorporate the above-mentioned electrochemical behavior,using the unique redox properties characteristic of triruthenium clusters:(i) each Ru_3 cluster unit generally exhibits four reversible single electron waves from Ru_3~(IV,III,III) to Ru_3~(II,II,II) state;(ii) the redox potentials of the cluster units strongly depend on the basicity of the ancillary ligand;(iii) redox potentials of the Ru_3 cluster units vary by 300-500 mV depending on the presence or the absence of a carbonyl ligand on the cluster unit;(iv) in the negative potential region,electronic interaction through the bridging pyrazine between adjacent Ru3 units containing a carbonyl ligand makes the difference in redox potential of each unit larger.1 and 2 were synthesized by linking Ru_3 cluster units with the desired ancillary ligand set in the appropriate order.
机译：三钌簇的吡嗪桥三聚体和四聚体低聚物，[{Ru_3O（CH_3CO_2）_6（（CO）（py）}-（mu-pz）-{Ru_3O（CH_3CO_2）_6（CO）}-（mu-pz）- {Ru_3O（CH_3CO_2）_6（py）_2}]〜+（1）和[{Ru_3O（CH_3CO_2）_6（CO）（py）}-（mu-pz）-{Ru_3O-（CH_3CO_2）_6（CO）} -（mu-pz）-{Ru_3O（CH_3CO_2）_6（Py））-（mu-pz）-{Ru_3O（CH_3CO_2）_6（dmap）_2}]〜（2+）（2），准备好了（pz =三聚体1和四聚体2在CH_3CN中的循环伏安图中分别显示出紧密间隔开的11步12电子和14步15电子可逆氧化还原波。根据三钌簇的独特氧化还原特性进行了专门设计以结合上述电化学行为：（i）每个Ru_3簇单元通常表现出从Ru_3〜（IV，III，III）到Ru_3〜（II）的四个可逆单电子波，II，II）状态;（ii）簇单元的氧化还原电势很大程度上取决于辅助配体的碱性;（iii）R的氧化还原电势u_3簇单元的变化幅度为300-500 mV，具体取决于簇单元上是否存在羰基配体;（iv）在负电势区域中，相邻的含羰基配体的Ru3单元之间通过桥连吡嗪的电子相互作用使得通过以适当的顺序将Ru_3簇单元与所需的辅助配体组连接，合成了每个单元的氧化还原电位差异较大。1和2。

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