In this project, we will use a combined experimental and theoretical approach in order to address three ambitious research topics. The common ground for these three sub-projects is the use of the highly reactive “Ni(diphosphine)” Ni(0) 14 electron fragment. The first sub-chapter addresses the current challenge of developing cross-coupling processes between C-sp3 (alkyl-halides) and organometallic compounds with first row transition metals. Preliminary results prove the Ni(diphosphine) fragment to be competent in such catalytic process, being the first example of its kind. The second project deals with the dehydrogenation of alkanes into alkenes using homogeneous catalysts. This very challenging task has never been reported with first row transition metal systems. Preliminary results indicate a stoichiometric transformation of the alkane by the above mentioned Ni fragment, opening the way for further improvements, and catalytic extension using different strategies (use of sacrificial alkene, use of tandem catalysis…). The third experimental project deals with CO2 functionalization. One of the originalities of our proposal is the design of the optimal Ni fragment for each process by theoretical calculations. This optimization step will only be possible after a comparison between experiments and theory for the known Ni(diphosphine) fragment.