Engineering of Ruthenium–Iron Oxide Colloidal Heterostructures: Improved Yields in CO2 Hydrogenation to Hydrocarbons. (17th October 2019)

• Record Type: Journal Article
• Authors: Aitbekova, Aisulu; Goodman, Emmett D.; Wu, Liheng; Boubnov, Alexey; Hoffman, Adam S.; Genc, Arda; Cheng, Huikai; Casalena, Lee; Bare, Simon R.; Cargnello, Matteo
• Is Part Of: Angewandte Chemie. Volume 131:Number 48(2019)
• Page Start: 17612
• Page End: 17618
• Publication Date: 2019-10-17
• Subjects: CO2-Hydrierung -- Eisen -- Kohlenwasserstoffe -- Ruthenium -- Wasserstoff-Spillover; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.201910579
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: Catalytic CO2 reduction to fuels and chemicals is a major pursuit in reducing greenhouse gas emissions. One approach utilizes the reverse water‐gas shift reaction, followed by Fischer–Tropsch synthesis, and iron is a well‐known candidate for this process. Some attempts have been made to modify and improve its reactivity, but resulted in limited success. Now, using ruthenium–iron oxide colloidal heterodimers, close contact between the two phases promotes the reduction of iron oxide via a proximal hydrogen spillover effect, leading to the formation of ruthenium–iron core–shell structures active for the reaction at significantly lower temperatures than in bare iron catalysts. Furthermore, by engineering the iron oxide shell thickness, a fourfold increase in hydrocarbon yield is achieved compared to the heterodimers. This work shows how rational design of colloidal heterostructures can result in materials with significantly improved catalytic performance in CO2 conversion processes. Abstract : Ruthenium fördert die Reduktion von Eisenoxid in Ruthienium‐Eisenoxid‐Heterodimeren durch einen proximalen Wasserstoff‐Spillover‐Effekt, was zur Bildung von Ruthenium‐Eisen‐Kern/Schalen‐Strukturen führt, die aktiv in der Hydrierung von CO2 zu Kohlenwasserstoffen sind. Die Feinabstimmung der Schalendicke führt zu einer vierfach höheren Kohlenwasserstoff‐Ausbeute.