Reactivity of Bis(pyridyl)-N-alkylaminato Methylpalladium Complexes toward Ethylene: Insights from Experiment and Theory

A series of novel neutral and cationic methylpalladium complexes bearing N-alkyl-2,2'-dipyridylaldiminato ligands were prepared and characterized. In the presence of ethylene, the cationic complexes were active as dimerization catalysts, producing a mixture of 1- and 2-butenes. A Pd-ethyl pi-ethylene species was identified as the catalyst resting state by low-temperature spectroscopic and DFT studies, which provided insights into the effect of both steric and electronic factors on the observed reactivity.