Abstract
The IrIII hydride (tBuPCN)IrHCl (1) containing the tridendate unsymmetrical pincer ligand tBuPCN– {tBuPCN(H) = 1-[3-[(di-tert-butylphosphino)methyl]phenyl]-1H-pyrazole} has been exploited as ammonia borane (NH3BH3, AB) and amine boranes dehydrogenation catalyst in THF solution at ambient temperature. 1 releases one H2 equivalent per AB equivalent, with concomitant cyclic poly(aminoboranes) formation [B-(cyclotriborazanyl)-amine-borane (BCTB) and cyclotriborazane (CTB)] as the final “spent fuel”. 1 has been found to have superior catalytic activity than its symmetrical analogue (tBuPCP)IrHCl, with recorded TOF values of 580 h–1 (AB in THF) and 401 h–1 (DMAB in toluene) at ambient temperature. The reaction has been analyzed experimentally through multinuclear [11B, 31P{1H}, 1H] NMR and IR spectroscopy, kinetic rate measurements, and kinetic isotope effect determination with deuterated AB isotopologues. The hydride/borohydride intermediate (tBuPCN)IrH(η2-BH4) (2) is the catalyst resting state formed during t...
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