Dataset Information

Metalloradical Reactivity of RuI and Ru0 Stabilized by an Indole-Based Tripodal Tetraphosphine Ligand.

ABSTRACT: The tripodal, tetradentate tris(1-(diphenylphosphanyl)-3-methyl-1H-indol-2-yl)phosphane PP3 -ligand 1 stabilizes Ru in the RuII , RuI , and Ru0 oxidation states. The octahedral [(PP3 )RuII (Cl)2 ]?(2), distorted trigonal bipyramidal [(PP3 )RuI (Cl)]?(3), and trigonal bipyramidal [(PP3 )Ru0 (N2 )]?(4) complexes were isolated and characterized by single-crystal X-ray diffraction, NMR, EPR, IR, and ESI-MS. Both open-shell metalloradical RuI complex 3 and the closed-shell Ru0 complex 4 undergo facile (net) abstraction of a Cl atom from dichloromethane, resulting in formation of the corresponding RuII and RuI complexes 2 and 3, respectively.

SUBMITTER: van de Watering FF

PROVIDER: S-EPMC5639366 | biostudies-literature | 2017 Sep

REPOSITORIES: biostudies-literature

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Metalloradical Reactivity of RuI and Ru0 Stabilized by an Indole-Based Tripodal Tetraphosphine Ligand.

van de Watering Fenna F FF van der Vlugt Jarl Ivar JI Dzik Wojciech I WI de Bruin Bas B Reek Joost N H JNH

Chemistry (Weinheim an der Bergstrasse, Germany) 20170830 52

The tripodal, tetradentate tris(1-(diphenylphosphanyl)-3-methyl-1H-indol-2-yl)phosphane PP3 -ligand 1 stabilizes Ru in the RuII , RuI , and Ru0 oxidation states. The octahedral [(PP3 )RuII (Cl)2 ] (2), distorted trigonal bipyramidal [(PP3 )RuI (Cl)] (3), and trigonal bipyramidal [(PP3 )Ru0 (N2 )] (4) complexes were isolated and characterized by single-crystal X-ray ...[more]

PMID: 28857278

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Project description:Seedless, surfactantless and support-free unprotected, metallic, interconnected nano-chain networks of ruthenium nanoparticles (NPs) were successfully synthesized via the reduction of ruthenium(iii) chloride (RuCl3) with sodium borohydride (NaBH4) at three different temperatures, viz. 30 °C, 45 °C and 60 °C. The molar ratio of RuCl3 solution and borohydride was optimized to be 1 : 1.5 to produce stable colloids with the optimum final solution pH of 9.7 ± 0.2. Average diameters of the interconnected nano-chain networks prepared at 30 °C (Ru-30), 45 °C (Ru-45) and 60 °C (Ru-60) were 3.5 ± 0.5 nm, 3.0 ± 0.2 nm and 2.6 ± 0.2 nm respectively. The morphology and composition dependent catalytic and electrocatalytic activities of these unprotected Ru nano-chain networks (Ru-30, Ru-45 and Ru-60) were studied in detail. The catalysis study was performed by investigating the transfer hydrogenation of several substituted aromatic nitro compounds. It was observed that Ru-60 was relatively more active compared to Ru-30 and Ru-45, which was reflected in their rate constant values. The electrocatalytic activities of Ru-30, Ru-45 and Ru-60 were screened for anodic water splitting in alkaline medium (0.1 M NaOH) and it was found that all of them showed almost the same activity which required an over-voltage of 308 ± 2 mV to obtain an anodic current density of 10 mA cm-2. The catalytic and electrocatalytic performances of these unprotected Ru0 networks were compared with Ru0 nanomaterials prepared under similar conditions with three different surfactants, viz. CTAB, SDS and TX-100, which revealed that unprotected Ru0 networks are better catalysts than those stabilized with surfactants. The superior catalytic and electrocatalytic performance is due to the availability of unprotected Ru0 surfaces. The present route may provide a new possibility of synthesizing other surfactant-free, unprotected metal colloids for enhanced catalytic and electrocatalytic applications.

Dataset Information

Metalloradical Reactivity of RuI and Ru0 Stabilized by an Indole-Based Tripodal Tetraphosphine Ligand.

Publications

Metalloradical Reactivity of Ru<sup>I</sup> and Ru<sup>0</sup> Stabilized by an Indole-Based Tripodal Tetraphosphine Ligand.

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