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Title: Active phase distribution changes within a catalyst particle during Fischer–Tropsch synthesis as revealed by multi-scale microscopy

In this study, the Fischer-Tropsch synthesis (FTS) reaction is one of the most promising processes to convert alternative energy sources, such as natural gas, coal or biomass, into liquid fuels and other high-value products. Despite its commercial implementation, we still lack fundamental insights into the various deactivation processes taking place during FTS. In this work, a combination of three methods for studying single catalyst particles at different length scales has been developed and applied to study the deactivation of Co/TiO 2 Fischer-Tropsch synthesis (FTS) catalysts. By combining transmission X-ray microscopy (TXM), scanning transmission X-ray microscopy (STXM) and scanning transmission electron microscopy-electron energy loss spectroscopy (STEM-EELS) we visualized changes in the structure, aggregate size and distribution of supported Co nanoparticles that occur during FTS. At the microscale, Co nanoparticle aggregates are transported over several μm leading to a more homogeneous Co distribution, while at the nanoscale Co forms a thin layer of ~1-2 nm around the TiO 2 support. The formation of the Co layer is the opposite case to the “classical” strong metal-support interaction (SMSI) in which TiO 2 surrounds the Co, and is possibly related to the surface oxidation of Co metal nanoparticles in combination with coke formation. Inmore » other words, the observed migration and formation of a thin CoO x layer are similar to a previously discussed reaction-induced spreading of metal oxides across a TiO 2 surface.« less
Authors:
 [1] ;  [2] ;  [3] ;  [3] ;  [4] ;  [1] ;  [1] ;  [1]
  1. Utrecht Univ., Utrecht (The Netherlands)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. Univ. Paris Sud, Orsay (France)
  4. Canadian Light Source, Saskatoon (Canada)
Publication Date:
Grant/Contract Number:
VICI, AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Catalysis Science and Technology
Additional Journal Information:
Journal Volume: 1021; Journal Issue: C; Journal ID: ISSN 2044-4753
Publisher:
Royal Society of Chemistry
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1251402

Cats, K. H., Andrews, J. C., Stephan, O., March, K., Karunakaran, C., Meirer, F., de Groot, F. M. F., and Weckhuysen, B. M.. Active phase distribution changes within a catalyst particle during Fischer–Tropsch synthesis as revealed by multi-scale microscopy. United States: N. p., Web. doi:10.1039/C5CY01524C.
Cats, K. H., Andrews, J. C., Stephan, O., March, K., Karunakaran, C., Meirer, F., de Groot, F. M. F., & Weckhuysen, B. M.. Active phase distribution changes within a catalyst particle during Fischer–Tropsch synthesis as revealed by multi-scale microscopy. United States. doi:10.1039/C5CY01524C.
Cats, K. H., Andrews, J. C., Stephan, O., March, K., Karunakaran, C., Meirer, F., de Groot, F. M. F., and Weckhuysen, B. M.. 2016. "Active phase distribution changes within a catalyst particle during Fischer–Tropsch synthesis as revealed by multi-scale microscopy". United States. doi:10.1039/C5CY01524C. https://www.osti.gov/servlets/purl/1251402.
@article{osti_1251402,
title = {Active phase distribution changes within a catalyst particle during Fischer–Tropsch synthesis as revealed by multi-scale microscopy},
author = {Cats, K. H. and Andrews, J. C. and Stephan, O. and March, K. and Karunakaran, C. and Meirer, F. and de Groot, F. M. F. and Weckhuysen, B. M.},
abstractNote = {In this study, the Fischer-Tropsch synthesis (FTS) reaction is one of the most promising processes to convert alternative energy sources, such as natural gas, coal or biomass, into liquid fuels and other high-value products. Despite its commercial implementation, we still lack fundamental insights into the various deactivation processes taking place during FTS. In this work, a combination of three methods for studying single catalyst particles at different length scales has been developed and applied to study the deactivation of Co/TiO2 Fischer-Tropsch synthesis (FTS) catalysts. By combining transmission X-ray microscopy (TXM), scanning transmission X-ray microscopy (STXM) and scanning transmission electron microscopy-electron energy loss spectroscopy (STEM-EELS) we visualized changes in the structure, aggregate size and distribution of supported Co nanoparticles that occur during FTS. At the microscale, Co nanoparticle aggregates are transported over several μm leading to a more homogeneous Co distribution, while at the nanoscale Co forms a thin layer of ~1-2 nm around the TiO2 support. The formation of the Co layer is the opposite case to the “classical” strong metal-support interaction (SMSI) in which TiO2 surrounds the Co, and is possibly related to the surface oxidation of Co metal nanoparticles in combination with coke formation. In other words, the observed migration and formation of a thin CoOx layer are similar to a previously discussed reaction-induced spreading of metal oxides across a TiO2 surface.},
doi = {10.1039/C5CY01524C},
journal = {Catalysis Science and Technology},
number = C,
volume = 1021,
place = {United States},
year = {2016},
month = {2}
}