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

Journal Article · · Catalysis Science and Technology
DOI:https://doi.org/10.1039/C5CY01524C· OSTI ID:1251402
 [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)

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.

Research Organization:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
VICI, AC02-76SF00515
OSTI ID:
1251402
Journal Information:
Catalysis Science and Technology, Vol. 1021, Issue C; ISSN 2044-4753
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 32 works
Citation information provided by
Web of Science

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Capturing the Genesis of an Active Fischer-Tropsch Synthesis Catalyst with Operando X-ray Nanospectroscopy journal August 2018
In-situ X-Ray Absorption Near Edge Structure Spectroscopy of a Solid Catalyst using a Laboratory-Based Set-up journal January 2019
In Situ Local Temperature Mapping in Microscopy Nano‐Reactors with Luminescence Thermometry journal October 2019
Cobalt‐Iron‐Manganese Catalysts for the Conversion of End‐of‐Life‐Tire‐Derived Syngas into Light Terminal Olefins journal February 2018
Spatial and temporal exploration of heterogeneous catalysts with synchrotron radiation journal August 2018
X-ray physico-chemical imaging during activation of cobalt-based Fischer–Tropsch synthesis catalysts
  • Beale, Andrew M.; Jacques, Simon D. M.; Di Michiel, Marco
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 376, Issue 2110 https://doi.org/10.1098/rsta.2017.0057
journal November 2017
Capturing the Genesis of an Active Fischer-Tropsch Synthesis Catalyst with Operando X-ray Nanospectroscopy journal August 2018