A computational study to determine whether substituents make E(13)[triple bond, length as m-dash]nitrogen (E(13) = B, Al, Ga, In, and Tl) triple bonds synthetically accessible

一项计算研究旨在确定取代基是否能使 E(13)[三键,键长以 m-dash 表示]氮(E(13) = B、Al、Ga、In 和 Tl)三键在合成上易于获得。

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Abstract

This study theoretically determines the effect of substituents on the stability of the triple-bonded L-E(13)[triple bond, length as m-dash]N-L (E(13) = B, Al, Ga, In, and Tl) compound using the M06-2X/Def2-TZVP, B3PW91/Def2-TZVP, and B3LYP/LANL2DZ+dp levels of theory. Five small substituents (F, OH, H, CH(3) and SiH(3)) and four large substituents (SiMe(SitBu(3))(2), SiiPrDis(2), Tbt ([double bond, length as m-dash] C(6)H(2)-2,4,6-{CH(SiMe(3))(2)}(3)) and Ar* ([double bond, length as m-dash]C(6)H(3)-2,6-(C(6)H(2)-2,4,6-i-Pr(3))(2))) are used. Unlike other triply bonded L-E(13)[triple bond, length as m-dash]P-L, L-E(13)[triple bond, length as m-dash]As-L, L-E(13)[triple bond, length as m-dash]Sb-L and L-E(13)[triple bond, length as m-dash]Bi-L molecules that have been studied, the theoretical findings for this study show that both small (but electropositive) ligands and bulky substituents can effectively stabilize the central E(13)[triple bond, length as m-dash]N triple bond. Nevertheless, these theoretical observations using the natural bond orbital and the natural resonance theory show that the central E(13)[triple bond, length as m-dash]N triple bond in these acetylene analogues must be weak, since these E(13)[triple bond, length as m-dash]N compounds with various ligands do not have a real triple bond.

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