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FeII Hexa N-Heterocyclic Carbene Complex with a 528 ps Metal-to-Ligand Charge-Transfer Excited-State Lifetime
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-01-11 00:00:00 , DOI: 10.1021/acs.jpclett.7b02962 Pavel Chábera , Kasper S. Kjaer 1 , Om Prakash , Alireza Honarfar , Yizhu Liu , Lisa A. Fredin , Tobias C. B. Harlang , Sven Lidin , Jens Uhlig , Villy Sundström , Reiner Lomoth 2 , Petter Persson , Kenneth Wärnmark
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-01-11 00:00:00 , DOI: 10.1021/acs.jpclett.7b02962 Pavel Chábera , Kasper S. Kjaer 1 , Om Prakash , Alireza Honarfar , Yizhu Liu , Lisa A. Fredin , Tobias C. B. Harlang , Sven Lidin , Jens Uhlig , Villy Sundström , Reiner Lomoth 2 , Petter Persson , Kenneth Wärnmark
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The iron carbene complex [FeII(btz)3](PF6)2 (where btz = 3,3′-dimethyl-1,1′-bis(p-tolyl)-4,4′-bis(1,2,3-triazol-5-ylidene)) has been synthesized, isolated, and characterized as a low-spin ferrous complex. It exhibits strong metal-to-ligand charge transfer (MLCT) absorption bands throughout the visible spectrum, and excitation of these bands gives rise to a 3MLCT state with a 528 ps excited-state lifetime in CH3CN solution that is more than one order of magnitude longer compared with the MLCT lifetime of any previously reported FeII complex. The low potential of the [Fe(btz)3]3+/[Fe(btz)3]2+ redox couple makes the 3MLCT state of [FeII(btz)3]2+ a potent photoreductant that can be generated by light absorption throughout the visible spectrum. Taken together with our recent results on the [FeIII(btz)3]3+ form of this complex, these results show that the FeII and FeIII oxidation states of the same Fe(btz)3 complex feature long-lived MLCT and LMCT states, respectively, demonstrating the versatility of iron N-heterocyclic carbene complexes as promising light-harvesters for a broad range of oxidizing and reducing conditions.
中文翻译：
铁II六ň N-杂环卡宾络合物具有528个ps的金属-配体电荷转移激发态寿命
卡宾铁络合物[Fe II（btz）3 ]（PF 6）2（其中btz = 3,3'-二甲基-1,1'-bis（对甲苯基）-4,4'-bis（1,2 ，3-三唑-5-亚基））已经合成，分离并且表征为低旋转的亚铁配合物。它在整个可见光谱范围内都表现出很强的金属到配体电荷转移（MLCT）吸收带，这些带的激发在CH 3 CN溶液中产生3 MLCT状态，激发态寿命为528 ps ，超过一个与以前报道的任何Fe II配合物的MLCT寿命相比，其数量级更长。[Fe（btz）3 ] 3+的低电势/ [Fe（btz）3 ] 2+的氧化还原对使[Fe II（btz）3 ] 2+的3 MLCT状态成为有效的光还原剂，可以通过吸收整个可见光谱来产生。连同我们对这种复合物的[Fe III（btz）3 ] 3+形式的最新研究结果，这些结果表明，同一Fe（btz）3配合物的Fe II和Fe III氧化态具有长寿命的MLCT和LMCT分别说明了N-铁的多功能性杂环卡宾配合物在广阔的氧化和还原条件下具有广阔的前景。
更新日期：2018-01-11
中文翻译：
铁II六ň N-杂环卡宾络合物具有528个ps的金属-配体电荷转移激发态寿命
卡宾铁络合物[Fe II（btz）3 ]（PF 6）2（其中btz = 3,3'-二甲基-1,1'-bis（对甲苯基）-4,4'-bis（1,2 ，3-三唑-5-亚基））已经合成，分离并且表征为低旋转的亚铁配合物。它在整个可见光谱范围内都表现出很强的金属到配体电荷转移（MLCT）吸收带，这些带的激发在CH 3 CN溶液中产生3 MLCT状态，激发态寿命为528 ps ，超过一个与以前报道的任何Fe II配合物的MLCT寿命相比，其数量级更长。[Fe（btz）3 ] 3+的低电势/ [Fe（btz）3 ] 2+的氧化还原对使[Fe II（btz）3 ] 2+的3 MLCT状态成为有效的光还原剂，可以通过吸收整个可见光谱来产生。连同我们对这种复合物的[Fe III（btz）3 ] 3+形式的最新研究结果，这些结果表明，同一Fe（btz）3配合物的Fe II和Fe III氧化态具有长寿命的MLCT和LMCT分别说明了N-铁的多功能性杂环卡宾配合物在广阔的氧化和还原条件下具有广阔的前景。
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