Signaling Recognition Events with Fluorescent Sensors and Switches.

https://www.pure.ed.ac.uk/ws/files/78983703/20190122_Robertson_Photoredox_review_RSC_style_final.pdf

Photoredox catalysts based on earth-abundant metal complexes

Chiral mixed phosphorus/sulfur ligands 1−3 have been shown to be effective in enantioselective Rh-catalyzed dehydroamino acid hydrogenation and ketone hydrosilylation reactions (eqs 1, 2). After assaying the influence of the substituents at sulfur, the substituents on the ligand backbone, the relative stereochemistry within the ligand backbone, and the substituents at phosphorus, ligands 2c (R = 3,5-dimethylphenyl) and 3 were found to be optimal in the Rh-catalyzed hydrogenation of a variety of α-acylaminoacrylates in high enantioselectivity (89−97% ee). A similar optimization of the catalyst for the Rh-catalyzed hydrosilylation of ketones showed that ligand 3 afforded the highest enantioselectivities for a wide variety of aryl alkyl and dialkyl ketones (up to 99% ee). A model for asymmetric induction in the hydrogenation reaction is discussed in the context of existing models, based on the absolute stereochemistry of the products and the X-ray crystal structures of catalyst precursors and intermediates.

Application of Chiral Mixed Phosphorus/Sulfur Ligands to Enantioselective Rhodium-Catalyzed Dehydroamino Acid Hydrogenation and Ketone Hydrosilylation Processes

The mechanism of asymmetric hydrogenation catalyzed by a new effective catalyst, viz., a rhodium complex of (S,S)-1,2-bis(tert-butylmethylphosphino)ethane (BisP*), has been studied by multinuclear NMR. Hydrogenation of the precatalyst [Rh(BisP*)(nbd)]BF4 (8) at −20 °C in deuteriomethanol affords solvate complex [Rh(BisP*)(CD3OD)2]BF4 (9), which is, in turn, hydrogenated at −90 °C producing equilibrium amounts (20% at −95 °C) of [RhH2(BisP*)(CD3OD)2] (10)the first observable dihydride of a Rh(I) complex with a diphosphine ligand. Dihydride 10 is in equilibrium with 9 and dihydrogen, which was studied in the temperature interval from −100 to −50 °C, yielding thermodynamic parameters ΔH = −6.3 ± 0.2 kcal M-1 and ΔS = −23.7 ± 0.7 cal M-1 K-1. The hydrogenation of 9 is stereoselective:  two isomers 10a and 10b are produced in a ratio 10:1. Use of HD for the hydrogenation of 9 yields the isomers with deuterium cis and trans to the phosphine in a ratio 1.3 (±0.1):1. The thermodynamic parameters of the equilibriu...

Mechanism of asymmetric hydrogenation catalyzed by a rhodium complex of (S,S)-1,2-bis(tert-butylmethylphosphino)ethane. Dihydride mechanism of asymmetric hydrogenation

The photoluminescence of metal complexes has attracted much recent interest since it can be utilized for a variety of applications such as optical sensors and LEDs. Moreover, the emission behavior provides a probe for the investigation of photoreactions including artificial photosynthesis. In this review, emitting compounds are classified according to the nature of their excited states: metal-centered, ligand-to-metal charge transfer, metal-to-ligand charge transfer, ligand-to-ligand charge transfer, metal-to-metal charge transfer, ligand-centered (or intraligand), and intraligand charge transfer excited states. Complexes of transition metals (dn with n=0 – 10), main group metals (s2), lanthanides and actinides (fn) are included in our discussion. However, this review does not cover the photoluminescence of metal complexes comprehensively, but illustrates this subject by selected examples. The viewpoint is that of a coordination chemist and not of a spectroscopist. Accordingly, molecular complexes which emit under ambient conditions are preferably chosen.

Luminescent Metal Complexes: Diversity of Excited States

Decamethylrhenocene, (η5-C5Me5)2Re

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Decamethylrhenocene, (η5-C5Me5)2Re