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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/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, themore » 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.« 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:
OSTI Identifier:
1251402
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 Laboratory (SLAC), 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