Thesis

Carbon dioxide, the main greenhouse gas, is also an abundant carbon resource that can be converted into value-added chemicals. Although CO2 reduction using hydrogen is a conventional approach, it remains energy-intensive due to the high dissociation energy of the H–H bond. An alternative strategy relies on the use of inorganic hydrides, such as hydrosilanes and hydroboranes, whose Si–H and B–H bonds are more readily activated. These compounds enable CO2 reduction under milder conditions through a homogeneous catalytic hydrosilylation step. To establish a sustainable cycle, the hydrides are regenerated electrochemically from silyl chlorides. With the aim of large-scale implementation and continuous operation, this PhD project focuses on the immobilization of molecular catalysts onto conductive surfaces. The objective is to functionalize these catalysts with anchoring groups in order to optimize their activity and increase the density of active sites. Various chemical and electrochemical strategies will be investigated. The modified catalysts will be grafted onto conductive supports and characterized using physicochemical and electrochemical techniques. Finally, the performance of the immobilized systems will be evaluated in terms of activity, selectivity, and stability, and compared with that of their homogeneous counterparts to identify the most efficient architectures for CO2 valorization.