Abstract
A magnesium complex (1) featuring a bidentate aminopyridinato ligand is a remarkably selective catalyst for the dehydrocoupling of amine‐boranes. This reaction proceeds to completion with low catalyst loadings (1 mol %) under mild conditions (60 °C), exceeding previously reported s‐block systems in terms of selectivity, rate, and turnover number (TON). Mechanistic studies by in situ NMR analysis reveals the reaction to be first order in both catalyst and substrate. A reaction mechanism is proposed to account for these findings, with the high TON of the catalyst attributed to the bidentate nature of the ligand, which allows for reversible deprotonation of the substrate and regeneration of 1 as a stable resting state.
Highlights
The transition from fossil fuels to a sustainable global energy system is one of the key challenges of the 21st century
The complexes were investigated as catalysts for the dehydrocoupling of Me2NH·BH3
Magnesium complex 1 is an effective catalyst for the dehydrocoupling/dehydrogenation of Me2NH·BH3 and iPr2NH·BH3
Summary
The transition from fossil fuels to a sustainable global energy system is one of the key challenges of the 21st century. Investigated as storage materials rather than catalysts,[30,31,32,33] their lack of popularity may be due to poor selectivity and extended reaction times of, for example, 124 h (72 % conversion) with Me2NH·BH3 as a substrate, as reported for Group 1 bis-(trimethylsilyl)amides.[34] recent work is yielding more active systems.[35,36] Whilst Group 2 systems have shown greater activity towards more complex amineborane substrates,[37,38,39] it should be noted that some systems studied have subsequently been shown to exhibit “spontaneous” dehydrocoupling.[40] In contrast, the Me2NH·BH3 and. We present a detailed mechanistic investigation into this catalysis, including stoichiometric reactivity studies and kinetic measurements, and propose a catalytic cycle to account for these data
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