The photocatalytic CO2 reduction reaction (P-CO2RR) is one promising way to mitigate CO2 levels in the atmosphere and generate solar fuels such as carbon monoxide (CO), methanol (CH3OH), formic acid (HCOOH) in a way that is inexpensive and environmentally friendly. In nature, photosynthesis is the process that converts CO2 to useful high-energy compounds. It achieves this by a series of hydride transfers from the reduced form of nicotinamide adenine dinucleotide (NADH) to captured CO2 and is driven by sunlight. Mimicking natural photosynthesis, we investigate several catalytic systems composed of a new class of organo-hydride catalysts that accelerate the selective CO2 reduction to formate via a hydride transfer. This work is a significant step towards the selective electrochemical and photochemical reduction of CO2 in a biomimetic approach, using a metal-free catalyst composed of earth-abundant elements. The projects are divided into two main sections. First, this thesis will discuss the “dark” processes that study thermodynamics and kinetics of the CO2 reduction with the new class of hydrides and then the “light-induced” processes that study the photochemical regeneration of organo-hydrides
