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The synthesis of carbon-neutral/zero-carbon footprint fuels via solar thermochemical processes (?Solar Fuels?) represents a promising approach for the realization of a sustainable energy future. These high temperature processes (effected by concentrated solar technology) ?regenerate? streams of ?dead hydrogen? (H2O) and/or ?dead carbon?, CO2, through thermochemical Water (WS) and/or Carbon Dioxide Splitting (CDS) into H2 and CO respectively, after contact with oxygen-deficient, ?redox? materials that are thus re-oxidized. Subsequently thermal reduction of the material is applied, by raising the temperature at a higher level, thus establishing a two-step cycle. Solar CO and H2 can be converted into solar fuels through gas-to-liquid catalytic processes. In this work, we summarize Material and Reactor Technologies for the development of solar fuels.  The approach entails the identification of attractive candidate material families (exhibiting redox behavior) exploiting the potential of computational chemistry based on ab initio calculations. Subsequently the desired materials are synthesized employing advanced manufacturing methods to generate tailored compositions/architectures.  These are shaped into structured reactor forms via various techniques and their performance is assessed under realistic conditions in the lab and at in-house and field-based, solar testing facilities.   We acknowledge support of this work by NSRF project MIS 5002704 PROMETHEUS (Greece & EU ERDF).

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