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A Monomeric Aluminum Imide (Iminoalane) with Al-N Triple-Bonding: Bonding Analysis and Dispersion Energy
Joshua D Queen1, Sini Irvankoski2, James C Fettinger1
1Department of Chemistry, University of California, Davis, One Shields Avenue, Davis California, 95616, United States.
Abstract:
The reaction of :AlAr (Ar = C6H-2,6-(C6H2-2,4,6-Pr3)2-3,5-Pr2) with ArMe6N3 (ArMe6 = C6H3-2,6-(C6H2-2,4,6-Me3)2) in hexanes at ambient temperature gave the aluminum imide ArAlNArMe6 (1). Its crystal structure displayed short Al-N distances of 1.625(4) and 1.628(3) Å with linear (C-Al-N-C = 180°) or almost linear (C-Al-N = 172.4(2)°; Al-N-C = 172.5(3)°) geometries. DFT calculations confirm linear geometry with an Al-N distance of 1.635 Å. According to energy decomposition analysis, the Al-N bond has three orbital components totaling -1350 kJ mol-1 and instantaneous interaction energy of -551 kJ mol-1 with respect to :AlAr and ArMe6N̈:. Dispersion accounts for -89 kJ mol-1, which is similar in strength to one Al-N π-interaction. The electronic spectrum has an intense transition at 290 nm which tails into the visible region. In the IR spectrum, the Al-N stretching band is calculated to appear at ca. 1100 cm-1. In contrast, reaction of :AlAr with 1-AdN3 or Me3SiN3 gave transient imides that immediately reacted with a second equivalent of the azide to give ArAl[(NAd)2N2] (2) or ArAl(N3){N(SiMe3)2} (3).
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