Abstract
The synthesis of a new tripodal phosphine ligand, N(CH 2PEt 2) 3, N-TriPhos Et is reported, and the use of tripodal ligands of this type, N(CH 2PR 2) 3 (R = Ph, Et), in conjunction with ruthenium for the catalysed hydrogenation of dimethyl oxalate (DMO) is reported and contrasted with catalysis using the MeC(CH 2PPh 2) 3 (TriPhos Ph) ligand. A different order of reaction with respect to the DMO substrate is found, and the rate is slower. A study of the kinetics and mechanism of the hydrogenation of DMO with Ru(acac) 3/TriPhos Ph is described, along with the effect of different additives to the system. The performance of Ru(acac) 3/TriPhos Ph/Zn system with unactivated ester substrates is probed and found to proceed significantly slower. Finally, based upon experimental observations, a mechanism is proposed for ester hydrogenation using ruthenium catalysts with tripodal phosphine ligands.
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