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1CO2 UTILIZATION VALERY plex have led to the highest catalyst turnover figures for the photocatalytic dehydrogenation of alkanes to date. A large number of alkanes, cycloalkanes and butane were dehydrated at low temperatures in the presence of UV light. In situ spectroscopic investigations and control tests formed the basis for a better understanding of the system. However, photocatalytic dehydration with sunlight as the light source could not be achieved, nor could direct carbonylation. For the hydroformylation with CO2, a ruthenium-based ligane-supported catalyst system was successfully developed, which is cur- rently the best system for the hydroformylation of olefins with CO2 in its ac- tivity. With the newly developed catalyst system, the hydrogenation activity could be almost completely suppressed and high selectivities to aldehyde/ alcohol could be observed. In addition, it has been shown that the retro-water- gas-shift reaction, the conversion of CO2 to CO, is already taking place at 110 °C with this system. Immobilization tests showed that it was not pos- sible to immobilize the photocatalytically active catalyst, but that hetero- genization of the catalyst system for hydroformylation using the SILP (sup- ported-ionic-liquid-phase) concept was possible. The catalyst systems were investigated in kinetic experiments. Based on these investigations, a reac- tor concept was developed for photocatalytic dehydration with UV light. It turned out that due to the low efficiency of the UV lamps and the high en- ergy consumption associated with it, a reactor system powered by UV light is neither economically nor ecologically sensible. Accordingly, a reactor con- cept for photocatalytic dehydration with sunlight was developed. Two criti- cal points were identified: one was the area required for the reactor and the other was the safety concept for a pressure-operated glass reactor. However, both points can be addressed by appropriate choice of materials and reactor design. Finally, the new process was evaluated economically and ecological- ly. It has been shown that the new process is an extremely attractive process in economic terms, since the use of alkanes and CO2 as C1 building blocks results in cost-effective raw materials and at the same time in an expan- sion of the raw material base. On the other hand, the new process‘s energy consumption is considerably lower than that of the established technology due to the energy-efficient photocatalytic dehydration with sunlight. The life cycle assessment has shown that the new process also has an immense ecological improvement potential. In all environmental impact categories, the new method is better than the benchmark and a decrease of up to 70 % could be observed in the individual sustainability criteria. From an econom- ic and ecological point of view, the new process is therefore an interesting alternative to the conventional production of valeraldehyde, provided that dehydration takes place in sunlight. During the project period, however, it was not possible to identify a suitable catalyst active in photocatalytic dehy- dration with sunlight. 52PDF Image | Chemical Processes and Use of CO2
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