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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. [ABSTRACT FROM AUTHOR]

Group 1 salts containing carbazolido NNN pincer ligands are precatalysts for the dehydrogenation of Me2NH·BH3. NMR monitoring and DOSY studies show a heavy dependence on the metal and solvent, allowing in some cases selective formation of dehydrogenation products consistent with hydrogen liberation. [ABSTRACT FROM AUTHOR]

Keywords: amido ligands; dehydrocoupling; homogeneous catalysis; hydrogen storage; magnesium We would like to clarify that in the paper Webster et al. a pure sample of Me SB 2 sb NH-BD SB 3 sb was synthesised based on the data they presented, and any implication that their spectra may have been mis-assigned was incorrect. Amido ligands, dehydrocoupling, homogeneous catalysis, hydrogen storage, magnesium. [Extracted from the article]