thermochemical; redox; perovskite; ceria; syngas; DFT; water splitting; CO2 splitting; solar energy; solar fuel
Muhich Christopher L., Blaser Samuel, Hoes Marie C., Steinfeld Aldo (2018), Comparing the solar-to-fuel energy conversion efficiency of ceria and perovskite based thermochemical redox cycles for splitting H2O and CO2, in International Journal of Hydrogen Energy
, 43(41), 18814-18831.
Jacot R., Naik J. Madhusudhan, Moré R., Michalsky R., Steinfeld A., Patzke G. R. (2018), Reactive stability of promising scalable doped ceria materials for thermochemical two-step CO 2 dissociation, in Journal of Materials Chemistry A
, 6(14), 5807-5816.
Ezbiri M., Becattini V., Hoes M., Michalsky R., Steinfeld A. (2017), High Redox Capacity of Al-Doped La 1− x Sr x MnO 3− δ Perovskites for Splitting CO 2 and H 2 O at Mn-Enriched Surfaces, in ChemSusChem
, 10(7), 1517-1525.
Marxer Daniel, Furler Philipp, Takacs Michael, Steinfeld Aldo (2017), Solar thermochemical splitting of CO 2 into separate streams of CO and O 2 with high selectivity, stability, conversion, and efficiency, in Energy Environ. Sci.
Hoes Marie, Muhich Christopher L., Jacot Roger, Patzke Greta R., Steinfeld Aldo (2017), Thermodynamics of paired charge-compensating doped ceria with superior redox performance for solar thermochemical splitting of H 2 O and CO 2, in Journal of Materials Chemistry A
, 5(36), 19476-19484.
Jacot Roger, Moré René, Michalsky Ronald, Steinfeld Aldo, Patzke Greta R. (2017), Trends in the phase stability and thermochemical oxygen exchange of ceria doped with potentially tetravalent metals, in J. Mater. Chem. A
, 5(37), 19901-19913.
Clean and sustainable fuels for transportation are a central challenge of the 21st century. Solar-driven H2O and CO2 splitting thermochemical cycles employing metal oxide redox reactions offer an energetically efficient approach for generating H2 and CO (syngas) as a precursor of liquid hydrocarbon fuels. This proposal aims at advancing our fundamental understanding of the physical chemistry principles that govern the performance of metal oxide redox materials, so that we can design and optimize these materials for maximizing the solar-to-fuel energy conversion efficiency. The research involves analyzing the tradeoffs between the thermodynamics of nonstoichiometric redox reactions versus the kinetics of oxygen vacancy diffusion. An assessment of ceria-based materials as benchmark reference will be performed, targeting the optimization of CeO2 through cationic doping strategies. Novel perovskite-based materials will be examined to outline descriptors of their thermo-mechanical stability, redox capacity, and oxygen conduction kinetics. Systematic DFT-based computational screening of defined performance descriptors will be employed and experimentally validated through thermogravimetric analysis and solid state characterization.