heal.abstract |
The current thesis focuses on the catalytic hydrogenation of carbon dioxide (CO2) using
both thermal and plasma methods. The catalysts used for this thesis were: CeO2,
CeO2/CuO 10%, and CeO2/CuO 20% and the main focus was to assess their efficiency,
selectivity to valuable products and stability.
The thesis begins by exploring the theoretical background of CO2 emissions and
introducing the CO2 hydrogenation reaction and its possible pathways. After discussing
the possible products that can be acquired by the reaction, then the non-noble catalysts
that facilitated the reaction were analyzed. Particularly, cerium oxide (CeO2) and copperdoped cerium oxide (CeO2/CuO 10%, and CeO2/CuO 20%).
The materials used in the experiments include CO2, hydrogen (H2), and helium (He)
gases, along with the catalysts that have already been mentioned. The experiments were
separated into two categories: thermal and plasma. For the thermal experiments, a
conventional oven was used as a source of energy, while for the plasma experiments, a
plug-flow dielectric barrier discharge (DBD) plasma reactor was used.
For the thermal method, experiments were conducted in various temperatures, starting
from 20 °C and reaching 500 °C, to determine the temperature at which each catalyst
becomes active, and the reaction takes place. CeO2 was the weakest catalyst since it
demonstrated minimal CO2 conversion at lower temperatures. The reactants started to
convert at 500 °C. The introduction of CuO to CeO2 significantly enhanced catalytic
performance. CeO2/CuO 20% achieves the highest CO2 conversion rates, at the lowest
temperatures (300 °C). This improved catalytic behavior is because of the synergistic
effect of CuO, which creates more active sites for CO2 adsorption and improves the
reduction process.
For the plasma experiments, the CO2 conversion was stable as a function of time. The
variable that was examined was how the CO2 conversion was affected by the different
applied voltages. Without a catalyst, CO2 conversion increased with voltage, reaching up
to 16% at 10 kV. The addition of the catalysts significantly improved the conversion and
stability of plasma. CeO2/CuO 20% showed once again the best catalytic performance
achieving 26% conversion at 10 kV. The plasma method was proved to be a very efficient
method since in room temperature, we were able to accomplish an adequate conversion.
Catalytic hydrogenation of carbon dioxide via plug-flow dielectric barrier discharge
(DBD) plasma reactor
Asteriou Zoi, 07.2024 Page 5 of 79
A comparative analysis of the thermal and plasma methods revealed that plasma-assisted
CO2 hydrogenation offers distinct advantages, particularly in terms of energy efficiency
and catalytic activity at lower temperatures. The CeO2/CuO 20% catalyst appeared to
have the best performance in both methods.
The last part of the experiment was the stability tests on the CeO2/CuO 20% catalyst.
Firstly, the catalyst was reduced with H2 at 500°C and then it was tested under plasma
conditions at 10 kV. The results showed consistent CO2 conversion rates over extended
periods. This shows that the catalyst can be used for long-term plasma-assisted CO2
hydrogenation processes.
To sum up, this study highlights the importance of catalysts in CO2 utilization. Future
research should focus on finding the optimal plasma parameters such as voltage, gas flow
ratios as well as exploring new catalyst compositions. Future research could also
investigate whether the additional loading of CuO results in even better conversions.
Additionally, the long-term stability of the catalyst should be further examined in order
to conclude whether such a process could be scaled up.
Concluding, this thesis emphasizes how the catalytic hydrogenation of CO2under thermal
and plasma sources, combined with non-noble catalysts can efficiently convert a
pollutant to chemically valuable products. |
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