Mechanistic studies on the addition of hydrogen to iridaepoxide complexes with subsequent elimination of water

Chemical Science
Lauren E DoyleDenis M Spasyuk

Abstract

Iridium complexes of the PCsp2 P ligand in which the donors are linked by 2,3-benzo[b]thiophene groups engage in the cooperative activation of N2O and the resulting iridaepoxides can be treated with dihydrogen to effect elimination of water and regeneration of the starting iridium complex. The mechanism of the steps in this reaction have been investigated using low temperature NMR investigations that reveal H/D exchange processes that point to a highly reactive kinetic product of hydrogen addition to the iridaepoxide. This intermediate is also involved in the water elimination pathway, and model compounds have been synthesized to provide further evidence for the mechanistic proposals for water elimination. The adaptable donor properties of the PCsp2 P ligand framework, particularly the anchoring carbene donor, plays a significant role in the ability of these compounds to mediate the transformation of N2O in this way.

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Citations

Jan 30, 2019·Chemistry : a European Journal·Addison N DesnoyerPierre Kennepohl
Jan 13, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Anthony F HillJas S Ward
Jul 16, 2020·Chemistry, an Asian Journal·Hendrik Tinnermann, Rowan D Young
Jul 29, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Joel D SmithJavier Borau-Garcia
Mar 14, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Lauren E DoyleDavid W Bi
Sep 5, 2017·Chemistry : a European Journal·Patrick E RothsteinVlad M Iluc
Oct 28, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Simon Sung, Rowan D Young
Oct 28, 2017·Chemistry : a European Journal·Dide G A VerhoevenMarc-Etienne Moret
Jul 28, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Dide G A Verhoeven, Marc-Etienne Moret
Jun 12, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Simon SungRowan D Young
Nov 17, 2016·Chemical Society Reviews·Addison N Desnoyer, Jennifer A Love
Jun 20, 2021·Angewandte Chemie·Qingyang WangRowan D Young

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Methods Mentioned

BETA
NMR
X-ray
co-crystallization

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