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Synthesis and Photochemical Properties of Re(I) Tricarbonyl Complexes Bound to Thione and Thiazol-2-ylidene Ligands
Organometallics ( IF 2.5 ) Pub Date : 2020-08-24 , DOI: 10.1021/acs.organomet.0c00381 Matthew J. Stout 1 , Brian W. Skelton 2 , Alexandre N. Sobolev 2 , Paolo Raiteri 3 , Massimiliano Massi 1 , Peter V. Simpson 1
Organometallics ( IF 2.5 ) Pub Date : 2020-08-24 , DOI: 10.1021/acs.organomet.0c00381 Matthew J. Stout 1 , Brian W. Skelton 2 , Alexandre N. Sobolev 2 , Paolo Raiteri 3 , Massimiliano Massi 1 , Peter V. Simpson 1
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Three Re(I) tricarbonyl complexes, with the general formulation Re(N^L)(CO)3X (where N^L is a bidentate ligand containing a pyridine functionalized at position 2 with a thione or a thiazol-2-ylidene group and X is either chloro or bromo), were synthesized and their reactivities explored in terms of solvent-dependent ligand substitution, in both the ground and excited states. When they were dissolved in acetonitrile, the complexes bound to the thione ligand underwent reversible ligand exchange with the solvent, resulting in the formation of Re(NCMe)2(CO)3X; the starting complex could be re-formed by precipitation following addition of diethyl ether. On the other hand, the complexes appeared to be inert in dichloromethane or acetone. Conversely, the complex bound to the thiazol-2-ylidene ligand did not display any ligand exchange reaction in the dark but underwent photoactivated ligand substitution on excitation to its lowest metal to ligand charge transfer manifold. Photolysis of this complex in acetonitrile generated multiple products, including Re(I) tricarbonyl and dicarbonyl solvato complexes as well as free thiazol-2-ylidene ligand.
中文翻译：
硫杂和噻唑-2-亚烷基配体上结合的三羰基Re（I）配合物的合成及光化学性质
三种Re（I）三羰基配合物，通式为Re（N ^ L）（CO）3 X（其中N ^ L是双齿配体，其中含有在2位被硫酮或噻唑-2-亚烷基官能化的吡啶（X是氯或溴），合成后在基态和激发态下根据溶剂依赖性配体取代来研究其反应性。当它们溶解在乙腈中时，与硫酮配体结合的复合物与溶剂进行可逆的配体交换，从而形成Re（NCMe）2（CO）3X; 可以在加入二乙醚后通过沉淀来重新形成起始配合物。另一方面，络合物在二氯甲烷或丙酮中似乎是惰性的。相反，与噻唑-2-亚烷基配体结合的复合物在黑暗中不显示任何配体交换反应，但在激发至其最低的金属-配体电荷转移歧管时经历了光活化的配体取代。该络合物在乙腈中的光解产生多种产物，包括Re（I）三羰基和二羰基溶剂化物络合物以及游离的噻唑-2-亚烷基配体。
更新日期：2020-09-14
中文翻译：
硫杂和噻唑-2-亚烷基配体上结合的三羰基Re（I）配合物的合成及光化学性质
三种Re（I）三羰基配合物，通式为Re（N ^ L）（CO）3 X（其中N ^ L是双齿配体，其中含有在2位被硫酮或噻唑-2-亚烷基官能化的吡啶（X是氯或溴），合成后在基态和激发态下根据溶剂依赖性配体取代来研究其反应性。当它们溶解在乙腈中时，与硫酮配体结合的复合物与溶剂进行可逆的配体交换，从而形成Re（NCMe）2（CO）3X; 可以在加入二乙醚后通过沉淀来重新形成起始配合物。另一方面，络合物在二氯甲烷或丙酮中似乎是惰性的。相反，与噻唑-2-亚烷基配体结合的复合物在黑暗中不显示任何配体交换反应，但在激发至其最低的金属-配体电荷转移歧管时经历了光活化的配体取代。该络合物在乙腈中的光解产生多种产物，包括Re（I）三羰基和二羰基溶剂化物络合物以及游离的噻唑-2-亚烷基配体。
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