Terminal and Super‐Basic Parent Imides of Hafnium

Bhunia, Mrinal; Sandoval‐Pauker, Christian; Jafari, Mehrafshan G.; Grant, Lauren N.; Gau, Michael R.; Pinter, Balazs; Mindiola, Daniel J.

doi:10.1002/anie.202209122

Terminal and Super‐Basic Parent Imides of Hafnium

Journal Article · 29 September 2022 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202209122· OSTI ID:2422435

Bhunia, Mrinal ^[1]; Sandoval‐Pauker, Christian ^[2]; Jafari, Mehrafshan G. ^[3]; Grant, Lauren N. ^[3]; Gau, Michael R. ^[3]; Pinter, Balazs ^[2]; ^[3]

Department of Chemistry University of Pennsylvania Philadelphia PA 19104 USA; OSTI
Department of Chemistry and Biochemistry University of Texas at El Paso El Paso TX 79968 USA
Department of Chemistry University of Pennsylvania Philadelphia PA 19104 USA

Abstract

A dinuclear hafnium complex containing the parent imido ligand [(PN)(PNC)Hf=NH{μ₂‐K}]₂(2) (PN⁻=(N‐(2‐PⁱPr₂‐4‐methylphenyl)‐2,4,6‐Me₃C₆H₂; PNC²⁻=(N‐(2‐PⁱPr₂‐4‐methylphenyl)‐2,4,6‐CH₂Me₂C₆H₂), was prepared by reduction of the bisazide trans‐[(PN)₂Hf(N₃)₂] (1) with two equiv of KC₈. Encapsulation of K⁺in2with crown‐ether or cryptand affords the first discrete salt [K(encap)][(PN)(PNC)Hf≡NH] (encap=18‐crown‐6(THF)₂,3; 2,2,2‐Kryptofix,4), featuring a terminal parent imide and possessing some of the shortest Hf−N bond lengths known to date. DFT calculations revealed formation of2to proceed via an extremely basic monomeric nitrido, [(PN)₂Hf≡N]⁻(A), having a computed pK_BH+of ∼57 followed by heterolytic splitting of an inert 1,2‐CH bond of a benzylic methyl group across the Hf≡N triple bond inA. An electronic structure analysis revealsAto possess a covalent Hf≡N triple bond and of super‐basic character. We also showcase reactivity of the Hf≡NH bond with various electrophiles.

Research Organization:: Indiana Univ., Bloomington, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

DOE Contract Number:: FG02-07ER15893

OSTI ID:: 2422435

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 43 Vol. 61; ISSN 1433-7851

Publisher:: Wiley

Country of Publication:: United States

Language:: English

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