2018
DOI: 10.1002/chem.201705619
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Optimization of Synthetically Versatile Pyridylidene Amide Ligands for Efficient Iridium‐Catalyzed Water Oxidation

Abstract: The synthetic versatility of pyridylidene amide (PYA) ligands has been exploited to prepare and evaluate a diverging series of iridium complexes containing C,N-bidentate chelating aryl-PYA ligands for water oxidation catalysis. The phenyl-PYA lead structure 1 was modified (i) electronically through introduction of one, two, or three electron-donating methoxy substituents on the aryl ring, (ii) by incorporating long aliphatic chains to the pyridyl fragment of the PYA unit, and (iii) by altering the PYA position… Show more

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Cited by 32 publications
(50 citation statements)
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“…Very recently, they investigated the promoting effect of incorporating MeO-groups. 188,189 Macchioni and co-workers found that the simple Cp*Ir complex [Ir(Cp*)(H 2 O) 3 ] 2+ (30) showed faster catalysis than those bearing auxiliary chelating ligands. 190 Hetterscheid and Reek reported a series of NHC-ligand-coordinated half-sandwich Cp*Ir complexes (31) with both high TOF (1.5 s À1 ) and high TON (42000) by using Ce 4+ as the oxidant.…”
Section: Overview Of Molecular Water-oxidation Catalysts (Wocs)mentioning
confidence: 99%
“…Very recently, they investigated the promoting effect of incorporating MeO-groups. 188,189 Macchioni and co-workers found that the simple Cp*Ir complex [Ir(Cp*)(H 2 O) 3 ] 2+ (30) showed faster catalysis than those bearing auxiliary chelating ligands. 190 Hetterscheid and Reek reported a series of NHC-ligand-coordinated half-sandwich Cp*Ir complexes (31) with both high TOF (1.5 s À1 ) and high TON (42000) by using Ce 4+ as the oxidant.…”
Section: Overview Of Molecular Water-oxidation Catalysts (Wocs)mentioning
confidence: 99%
“…[44][45][46] The flexibility imparts catalytic activity, and is further modulated upon alteration of the pyridine substitution pattern from para-PYAs (A, B) to meta-PYA scaffolds (C, Scheme 1). 47 Of note, such meta-PYA ligands cannot be represented by a neutral resonance structure and feature only zwitterionic structures. 48 Provided resonance structures D-F are also relevant, then these ligands are mesoionic N-donor systems, 49 related to mesoionic N-heterocyclic carbenes.…”
Section: Introductionmentioning
confidence: 99%
“…Successively, many other molecular Ir WOCs were reported, and many excellent and exhaustive reviews recently appeared in the literature , , . Herein, the focus is on the stability and activity of Ir WOCs, two strictly interlocked and crucial aspects.…”
Section: Molecular Ir Wocsmentioning
confidence: 99%