Solar-driven H2O/CO2 conversion to fuels via two-step electro-thermochemical cycle in a solid oxide electrochemical cell

Ni-phyllosilicate nanotubes coated by CeO2 for ultra-efficiency of 36.9% in solar-driven conversion of CO2-to-fuel

MIL-68 (In)-derived In2O3@TiO2 S-scheme heterojunction with hierarchical hollow structure for selective photoconversion of CO2 to hydrocarbon fuels

The solar thermochemical two-step splitting of H2O and CO2 based on metal oxide compounds is a promising path for clean and efficient generation of hydrogen and renewable synthetic fuels. The two-step process is based on the endothermic solar thermal reduction of a metal oxide releasing O2 using a high-temperature concentrated solar heat source, followed by the exothermic oxidation of the reduced oxide with H2O and/or CO2 to generate pure H2 and/or CO. This pathway relates to one of the emerging and most promising processes for solar thermochemical fuel production encompassing green H2 and the recycling/valorization of anthropogenic greenhouse gas emissions. It represents an efficient route for solar energy conversion and storage into renewable and dispatchable fuels, by directly converting the whole solar spectrum using heat delivered by concentrating systems. This eliminates the need for photocatalysts or intermediate electricity production, thus bypassing the main limitations of the low-efficient photochemical and electrochemical routes currently seen as the main green methods for solar fuel production. In this context, among the relevant potential redox materials, thermochemical cycles based on volatile and non-volatile metal oxides are particularly attractive. Most redox pairs in two-step cycles proceed with a phase change (solid-to-gas or solid-to-liquid) during the reduction step, which can be avoided by using non-stoichiometric oxides (chiefly, spinel, fluorite, or perovskite-structured materials) through the creation of oxygen vacancies in the lattice. The oxygen sub-stoichiometry determines the oxygen exchange capacity, thus determining the fuel production output per mass of redox-active material. This paper provides an overview of the most advanced cycles involving ZnO/Zn, SnO2/SnO, Fe3O4/FeO, ferrites, ceria, and perovskites redox systems by focusing on their ability to perform H2O and CO2 splitting during two-step thermochemical cycles with high fuel production yields, rapid reaction rates, and performance stability. Furthermore, the possible routes for redox-active material integration and processing in various solar reactor technologies are also described.

/pdf/redox-cycles-active-materials-and-reactors-applied-to-water-3fvv390k.pdf

Redox Cycles, Active Materials, and Reactors Applied to Water and Carbon Dioxide Splitting for Solar Thermochemical Fuel Production: A Review

Direct solar thermochemical CO2 splitting based on Ca- and Al- doped SmMnO3 perovskites: Ultrahigh CO yield within small temperature swing

Solar thermochemical CO2-to-fuel conversion via two-step redox cycles is a promising strategy to solve climate change and energy storage challenges simultaneously. However, ideal thermochemical materials possessing moderate operation temperature, high yield, good stability, and rapid kinetics operating under isothermal and near-isothermal conditions are still missing. Here, we propose Sr-doped SmMnO3 for moderate-temperature near-isothermal CO2-to-fuel conversions. A record-high isothermal cycle CO yield (376.1 μmol g−1) at no more than 1300 °C is reported based on Sm0.6Sr0.4MnO3. No obvious decay is observed during 14 cycles although grain sizes have increased to some extent. The weakened Mn–O bond induced by Sr doping helps to create more oxygen vacancies, and thus contributes to enhanced yield of both O2 and CO. The oxidation reaction is fast with a CO yield of 58.6 μmol g−1 in 15 minutes, which is 5.6 times as high as that of CeO2 under the same cycling conditions between 1300 °C and 1000 °C. Detailed kinetics for the oxidation step is unveiled based on the Sestak–Berggren model. In addition, SmxSr1−xMnO3 can capture full-spectrum solar energy with a solar absorptance of more than 86.6% in stark contrast to 13.5% for CeO2, making the required concentration ratio to drive reactions decrease by 33.4%. This work provides new materials for high yield and stable thermochemical CO2-to-fuel conversion under moderate-temperature near-isothermal conditions, and paves the way for the development of CO2 splitting techniques directly driven by low-concentration solar energy with high efficiencies.

Sr-doped SmMnO3 perovskites for high-performance near-isothermal solar thermochemical CO2-to-fuel conversion

Highly efficient solar-driven CO2-to-fuel conversion assisted by CH4 over NiCo-ZIF derived catalysts

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Sr-doped SmMnO3 perovskites for high-performance near-isothermal solar thermochemical CO2-to-fuel conversion

Highly efficient solar-driven CO2-to-fuel conversion assisted by CH4 over NiCo-ZIF derived catalysts