Engineering of Ruthenium-Iron Oxide Colloidal Heterostructures: Improved Yields in CO2 Hydrogenation to Hydrocarbons

Aitbekova, Aisulu; Goodman, Emmett D.; Wu, Liheng; Boubnov, Alexey; Hoffman, Adam S.; Genc, Arda; Cheng, Huikai; Casalena, Lee; Bare, Simon R.; Cargnello, Matteo

doi:10.1002/anie.201910579

Title: Engineering of Ruthenium-Iron Oxide Colloidal Heterostructures: Improved Yields in CO₂ Hydrogenation to Hydrocarbons

Journal Article · 23 September 2019 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.201910579 · OSTI ID:1575223

Aitbekova, Aisulu ^[1]; Goodman, Emmett D. ^[1]; Wu, Liheng ^[2]; Boubnov, Alexey ^[3];

^[3]; Genc, Arda ^[4]; Cheng, Huikai ^[4]; Casalena, Lee ^[4];

^[3];

^[1]

Stanford Univ., Stanford, CA (United States). Dept. of Chemical Engineering and SUNCAT Center for Interface Science and Catalysis
Stanford Univ., Stanford, CA (United States). Dept. of Chemical Engineering and SUNCAT Center for Interface Science and Catalysis; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource
Thermo Fisher Scientific, Hillsboro, OR (United States)

Catalytic CO₂ reduction to fuels and chemicals is a major pursuit in reducing greenhouse gas emissions. Here, 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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1575223

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 48 Vol. 58; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2 hydrogenation
hydrocarbons
hydrogen spillover
iron
ruthenium

Title: Engineering of Ruthenium-Iron Oxide Colloidal Heterostructures: Improved Yields in CO2 Hydrogenation to Hydrocarbons

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Title: Engineering of Ruthenium-Iron Oxide Colloidal Heterostructures: Improved Yields in CO₂ Hydrogenation to Hydrocarbons