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The Synthesis, Characterization and Reactivity of a Series of Ruthenium N-triphosPh Complexes

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Published on: April 10, 2015

Oxygen Reduction with a Bifunctional Iridium Dihydride Complex.

Christoph Schiwek¹, Jenni Meiners¹, Moritz Förster²

¹Institut für Anorganische Chemie, Georg-August-Universität, Tammannstr. 4, 37077 Göttingen (Germany).

Angewandte Chemie (International Ed. in English)

|October 30, 2015

Summary

A novel iridium dihydride complex facilitates a synthetic oxygen-reduction reaction (ORR) by storing four electrons in metal-hydride bonds. This discovery offers a new pathway for efficient oxygen reduction using homogeneous catalysts.

Keywords:

density functional calculations hydrides iridium oxygen pincer ligands

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Area of Science:

Inorganic Chemistry
Organometallic Chemistry
Catalysis

Background:

The oxygen-reduction reaction (ORR) is crucial in energy conversion but challenging to achieve efficiently with homogeneous catalysts.
Mononuclear metal complexes with M-H bonds offer potential for multi-electron transfer processes.

Purpose of the Study:

To investigate the reaction of an iridium dihydride complex with O2.
To elucidate the mechanism of oxygen reduction by a mononuclear iridium complex.
To demonstrate a quasi-catalytic ORR cycle.

Main Methods:

Synthesis and characterization of the iridium dihydride complex [Ir(H)2(PNP)]+.
Experimental studies of the reaction with O2 and H2.
Computational studies (e.g., DFT) to probe the reaction mechanism.

Main Results:

The iridium dihydride complex reacts with O2 to form an iridium(III) hydroxide species and water.
A quasi-catalytic ORR cycle was successfully demonstrated by regenerating the dihydride with H2.
Mechanism involves O2 coordination followed by H-transfer at the metal center, facilitated by the pincer ligand.

Conclusions:

Mononuclear iridium complexes with M-H bonds can store the four electrons required for ORR.
The pincer ligand plays a key role in facilitating the oxygenation and H-transfer steps.
This work presents a new synthetic route for ORR using homogeneous catalysis.