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Title: Engineering of Ruthenium-Iron Oxide Colloidal Heterostructures: Improved Yields in CO 2 Hydrogenation to Hydrocarbons

Abstract

Catalytic CO 2 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 CO 2 conversion processes.

Authors:
 [1];  [1];  [2];  [3]; ORCiD logo [3];  [4];  [4];  [4]; ORCiD logo [3]; ORCiD logo [1]
  1. Stanford Univ., Stanford, CA (United States). Dept. of Chemical Engineering and SUNCAT Center for Interface Science and Catalysis
  2. 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
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource
  4. Thermo Fisher Scientific, Hillsboro, OR (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1575223
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 58; Journal Issue: 48; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 hydrogenation; hydrocarbons; hydrogen spillover; iron; ruthenium

Citation Formats

Aitbekova, Aisulu, Goodman, Emmett D., Wu, Liheng, Boubnov, Alexey, Hoffman, Adam S., Genc, Arda, Cheng, Huikai, Casalena, Lee, Bare, Simon R., and Cargnello, Matteo. Engineering of Ruthenium-Iron Oxide Colloidal Heterostructures: Improved Yields in CO2 Hydrogenation to Hydrocarbons. United States: N. p., 2019. Web. doi:10.1002/anie.201910579.
Aitbekova, Aisulu, Goodman, Emmett D., Wu, Liheng, Boubnov, Alexey, Hoffman, Adam S., Genc, Arda, Cheng, Huikai, Casalena, Lee, Bare, Simon R., & Cargnello, Matteo. Engineering of Ruthenium-Iron Oxide Colloidal Heterostructures: Improved Yields in CO2 Hydrogenation to Hydrocarbons. United States. doi:10.1002/anie.201910579.
Aitbekova, Aisulu, Goodman, Emmett D., Wu, Liheng, Boubnov, Alexey, Hoffman, Adam S., Genc, Arda, Cheng, Huikai, Casalena, Lee, Bare, Simon R., and Cargnello, Matteo. Mon . "Engineering of Ruthenium-Iron Oxide Colloidal Heterostructures: Improved Yields in CO2 Hydrogenation to Hydrocarbons". United States. doi:10.1002/anie.201910579.
@article{osti_1575223,
title = {Engineering of Ruthenium-Iron Oxide Colloidal Heterostructures: Improved Yields in CO2 Hydrogenation to Hydrocarbons},
author = {Aitbekova, Aisulu and Goodman, Emmett D. and Wu, Liheng and Boubnov, Alexey and Hoffman, Adam S. and Genc, Arda and Cheng, Huikai and Casalena, Lee and Bare, Simon R. and Cargnello, Matteo},
abstractNote = {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.},
doi = {10.1002/anie.201910579},
journal = {Angewandte Chemie (International Edition)},
number = 48,
volume = 58,
place = {United States},
year = {2019},
month = {9}
}

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