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Towards noble-metal free dyads: Ground and excited state tuning by a cobalt dimethylglyoxime catalyst connected to an iron N-heterocyclic carbene photosensitizer
European Journal of Inorganic Chemistry ( IF 2.2 ) Pub Date : 2018-12-17 , DOI: 10.1002/ejic.201800946
Peter Zimmer 1 , Lukas Burkhardt 1 , Rahel Schepper 1 , Kaibo Zheng 2, 3 , David Gosztola 4 , Adam Neuba 1 , Ulrich Flörke 1 , Christoph Wölper 5 , Roland Schoch 1 , Wojciech Gawelda 6, 7 , Sophie E. Canton 8 , Matthias Bauer 1
Affiliation  

Heteroleptic iron based complexes bearing the 2,6-bis[3-(2,6-diisopropylphenyl)imidazol-2-ylidene]pyridine motif and a polypridine ligand have been synthesized and characterized in their ground and excited state. This series of complexes includes a first example of a hetero-bimetallic complex connecting an iron N-heterocyclic carbene photosensitizer with a cobalt dimethylglyoxime fragment. Focus is set on the influence of the linker and cobalt center as second ligand at the iron center on the photophysics. While electronic absorption spectroscopy and cyclic voltammetry reveal a weak mutual influence of the single ligands in the heteroleptic complexes, an increasing MLCT lifetime with larger π-accepting abilities was found by time-resolved transient absorption spectroscopy, with maximum lifetime in the case of the hetero-bimetallic dyad. Concurrently the MC lifetimes were observed to decrease. The reported results will allow to develop guidelines for designing bimetallic devices, which may allow electron transfer from the photosensitizer fragment to a catalytically active center. (Less)

中文翻译:

走向不含贵金属的二元组:通过连接到铁 N-杂环卡宾光敏剂的钴二甲基乙二肟催化剂进行基态和激发态调谐

已经合成了带有 2,6-双[3-(2,6-二异丙基苯基)咪唑-2-亚基]吡啶基序和多吡啶配体的杂配铁基配合物,并在它们的基态和激发态下进行了表征。这一系列配合物包括将铁 N-杂环卡宾光敏剂与钴二甲基乙醛肟片段连接的异双金属配合物的第一个例子。重点是连接子和钴中心作为铁中心的第二配体对光物理的影响。虽然电子吸收光谱和循环伏安法揭示了杂配配合物中单个配体的微弱相互影响,但时间分辨瞬态吸收光谱发现 MLCT 寿命增加,π 接受能力更大,在杂配体的情况下寿命最大-双金属二元组。同时观察到 MC 寿命减少。报告的结果将允许制定双金属器件的设计指南,这可能允许电子从光敏剂片段转移到催化活性中心。(较少的)
更新日期:2018-12-17
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