Abstract
For a more environmentally friendly process, the hydrogenation of biosourced platform molecules such as succinic acid has to be carried out in the aqueous phase. Considering the harsh reaction conditions (160 °C, 150 bars H2, acid aqueous medium), the design of new, highly stable catalysts is needed. The most active and selective catalysts described for the aqueous phase hydrogenation of succinic acid to 1,4-butanediol are based on palladium promoted by rhenium, impregnated on a TiO2 anatase support. In this thesis, the non-hydrolytic sol-gel process has been used to prepare different oxide and mixed oxide supports based on TiO2 and ZrO2, which are the most stable oxides under hydrothermal conditions. This process allowed the one-step synthesis of high specific surface area mesoporous supports with a controlled crystalline structure and composition. In particular, we showed that it was possible to prepare “promoted supports” (TiO2-Re2O7, TiO2-MoO3, ZrO2-Re2O7, ZrO2-MoO3), incorporating the transition metal promoter, which migrates toward the surface during the calcination. Our hypothesis was that this approach would lead to a better dispersion and possibly a better stability of the promoter, and thus to a more efficient catalyst. The first catalytic tests carried out by our partners at IRCELYON showed that the Pd-based catalysts obtained with our promoted TiO2 supports were more selective and more active than the equivalent catalysts prepared by impregnation from Pd. Then the promoter on a TiO2 support, which seems to validate our initial hypothesis. Catalysis tests on the promoted ZrO2 and ZrO2 substrates are ongoing.