Design principles of perovskites for solar-driven thermochemical splitting of CO.

Perovskites are attractive redox materials for thermo/electrochemical fuel synthesis. To design perovskites with balanced redox energetics for thermochemically splitting CO, the activity of lattice oxygen vacancies and stability against crystal phase changes and detrimental carbonate formation are predicted for a representative range of perovskites by electronic structure computations. Systematic trends in these materials properties when doping with selected metal cations are described in the free energy range defined for isothermal and temperature-swing redox cycles.

Solar-Driven Thermochemical Splitting of CO and Separation of CO and O across a Ceria Redox Membrane Reactor.

Splitting CO with a thermochemical redox cycle utilizes the entire solar spectrum and provides a favorable path to the synthesis of solar fuels at high rates and efficiencies. However, the temperature/pressure swing commonly applied between reduction and oxidation steps incurs irreversible energy losses and severe material stresses. Here, we experimentally demonstrate for the first time the single-step continuous splitting of CO into separate streams of CO and O under steady-state isothermal/isobaric conditions.

Tunable thermodynamic activity of La Sr Mn Al O (0 ≤ ≤ 1, 0 ≤ ≤ 1) perovskites for solar thermochemical fuel synthesis.

Nonstoichiometric metal oxides with variable valence are attractive redox materials for thermochemical and electrochemical fuel processing. To guide the design of advanced redox materials for solar-driven splitting of CO and/or HO to produce CO and/or H (syngas), we investigate the equilibrium thermodynamics of the La Sr Mn Al O perovskite family (0 ≤ ≤ 1, 0 ≤ ≤ 1) and LaCaMnAlO , and compare them to those of CeO as the baseline. Oxygen nonstoichiometry measurements from 1573 to 1773 K and from 0.

High Redox Capacity of Al-Doped La Sr MnO Perovskites for Splitting CO and H O at Mn-Enriched Surfaces.

Perovskites are attractive candidates for the solar-driven thermochemical redox splitting of CO and H O into CO and H (syngas) and O . This work investigates the surface activity of La Sr Mn Al O (0≤x≤1, 0≤y≤1) and La Ca Mn Al O . At 1623 K and 15 mbar O , the oxygen non-stoichiometry of La Sr Mn Al O increases with the strontium content and reaches a maximum of δ=0.