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Enantioenriched Ruthenium-Tris-Bipyridine Complexes Bearing One Helical Bipyridine Ligand: Access to Fused Multihelicenic Systems and Chiroptical Redox Switches
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2021-07-23 , DOI: 10.1021/acs.inorgchem.1c01379 Martin Kos 1 , Rafael Rodríguez 2 , Jan Storch 1 , Jan Sýkora 1 , Elsa Caytan 2 , Marie Cordier 2 , Ivana Císařová 3 , Nicolas Vanthuyne 4 , J A Gareth Williams 5 , Jaroslav Žádný 1 , Vladimír Církva 1 , Jeanne Crassous 2
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2021-07-23 , DOI: 10.1021/acs.inorgchem.1c01379 Martin Kos 1 , Rafael Rodríguez 2 , Jan Storch 1 , Jan Sýkora 1 , Elsa Caytan 2 , Marie Cordier 2 , Ivana Císařová 3 , Nicolas Vanthuyne 4 , J A Gareth Williams 5 , Jaroslav Žádný 1 , Vladimír Církva 1 , Jeanne Crassous 2
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The synthesis and photophysical and chiroptical properties of novel aza[n]helicenes (6a–d, 10a,b, n = 4–7) substituted with one or two 2-pyridyl groups are described. The preparation was performed via an adapted Mallory reaction using aromatic imines as precursors. The obtained novel class of helical 2,2′-bipyridine ligands was then coordinated to Ru(bipy)22+ units, thus affording the first diastereomerically and enantiomerically pure [RuL(bipy)2]2+ (11a,c, L = 6a,c) or [Ru2L′(bipy)4]4+ (12, L′ = 10b) complexes. The topology and stereochemistry of these novel metal-based helical architectures were studied in detail, notably using X-ray crystallography. Interestingly, the coordination to ruthenium(II) enabled the preparation of fused multihelical systems incorporating aza- and ruthena-helicenes within the same scaffold. The photophysical, chiroptical, and redox properties of these complexes were examined in detail, and efficient redox-triggered chiroptical switching activity was evidenced.
中文翻译：
带有一个螺旋双吡啶配体的对映体富集的钌-三-联吡啶配合物：获得融合多螺旋系统和手性氧化还原开关
描述了被一个或两个 2-吡啶基取代的新型氮杂[ n ]螺旋烯（6a - d，10a，b，n = 4-7）的合成和光物理和手性光学特性。该制备是通过使用芳族亚胺作为前体的经过调整的 Mallory 反应进行的。然后将获得的新型螺旋 2,2'-联吡啶配体与 Ru(bipy) 2 2+单元配位，从而提供第一个非对映异构和对映异构纯 [RuL(bipy) 2 ] 2+ ( 11a , c , L = 6a , c ) 或 [Ru 2L'(bipy) 4 ] 4+ ( 12 , L' = 10b ) 复合物。详细研究了这些新型金属螺旋结构的拓扑结构和立体化学，特别是使用 X 射线晶体学。有趣的是，与钌 (II) 的配位使得能够在同一支架内制备包含氮杂-和钌-螺旋烯的融合多螺旋系统。详细检查了这些复合物的光物理、手性和氧化还原特性，并证明了有效的氧化还原触发的手性转换活性。
更新日期：2021-08-16
中文翻译：
带有一个螺旋双吡啶配体的对映体富集的钌-三-联吡啶配合物：获得融合多螺旋系统和手性氧化还原开关
描述了被一个或两个 2-吡啶基取代的新型氮杂[ n ]螺旋烯（6a - d，10a，b，n = 4-7）的合成和光物理和手性光学特性。该制备是通过使用芳族亚胺作为前体的经过调整的 Mallory 反应进行的。然后将获得的新型螺旋 2,2'-联吡啶配体与 Ru(bipy) 2 2+单元配位，从而提供第一个非对映异构和对映异构纯 [RuL(bipy) 2 ] 2+ ( 11a , c , L = 6a , c ) 或 [Ru 2L'(bipy) 4 ] 4+ ( 12 , L' = 10b ) 复合物。详细研究了这些新型金属螺旋结构的拓扑结构和立体化学，特别是使用 X 射线晶体学。有趣的是，与钌 (II) 的配位使得能够在同一支架内制备包含氮杂-和钌-螺旋烯的融合多螺旋系统。详细检查了这些复合物的光物理、手性和氧化还原特性，并证明了有效的氧化还原触发的手性转换活性。
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