Artificial Photosynthesis : Carbon dioxide photoreduction and catalyst heterogenization within solid materials

Abstract : In the context of global warming and the necessary substitution of renewable energies (solar and wind energy) for fossil fuels, efficient energy-storage technologies need to be urgently developed. Recently, energy storage via the reduction of CO2 has seen renewed interest. Although reduction of CO2 into energy-dense liquid or gaseous fuels is a fascinating fundamental issue, its practical implementation in technological devices is highly challenging due to the high stability of CO2 and thus the endergonic nature of its transformation. Furthermore, the reactions involve multiple electrons and protons and thus require efficient catalysts to mediate these transformations.The objective of this thesis is to investigate different strategies for the storage of solar energy in chemical compounds, through visible-light-driven CO2 reduction. This thesis comprises of two main parts. After an introduction, the first part describes the investigation of homogeneous catalysts in combination with a photosensitizer, either separately or connected covalently. Due to the easily-tunable synthesis and facile characterization of molecular catalysts, homogeneous photosystems are more controllable and can give deep insight into product selectivity and mechanistic issues.With regards to future applicability, however, homogeneous catalysis often suffers from additional costs associated with solvents, product isolation and catalyst recovery, amongst other factors. The integration of molecular catalysts into solid platforms offers the possibility to maintain the advantageous properties of homogeneous catalysts while moving towards practical system designs afforded by heterogeneous catalysis. The second part of this thesis is therefore the immobilization of molecular catalysts within solid materials, namely MOFs and PMO. The ultimate goal of this thesis is to incorporate both catalyst and photosensitizer into the solid support.
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Xia Wang. Artificial Photosynthesis : Carbon dioxide photoreduction and catalyst heterogenization within solid materials. Organic chemistry. PSL Research University, 2017. English. ⟨NNT : 2017PSLET025⟩. ⟨tel-02356179⟩

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