Two-fold proton coupled electron transfer of a Ta(V) aniline complex mediated by a redox active NNN pincer ligand

IF 3.5 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR
Sotirios Pavlidis, Jasmin Alasadi, Amanda Opis Basilio, Josh Abbenseth
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引用次数: 0

Abstract

We report the proton-coupled electron transfer (PCET) reactivity of an octahedral Ta(V) aniline complex supported by an acridane-derived redox-active NNN pincer ligand. The reversible binding of aniline to a Ta(V) dichloride induces significant coordination-induced bond weakening (CIBW) of the aniline N–H bonds. This enables a rare two-fold hydrogen atom abstraction, resulting in a terminal imido complex and a two-electron oxidation of the NNN pincer ligand, all while maintaining the metal's oxidation state. The bond dissociation free energies (BDFEs) of the aniline and a transient radical amido complex are estimated through stoichiometric reactions with different hydrogen atom abstractors and donors, further supported by density functional theory calculations.
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来源期刊
Dalton Transactions
Dalton Transactions 化学-无机化学与核化学
CiteScore
6.60
自引率
7.50%
发文量
1832
审稿时长
1.5 months
期刊介绍: Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.
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