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On the Origin of the Cobalt Particle Size Effects in Fischer−Tropsch Catalysis
Abstract
The effects of metal particle size in catalysis are of prime scientific and industrial importance and call for a better understanding. In this paper the origin of the cobalt particle size effects in Fischer-Tropsch (FT) catalysis was studied. Steady-State Isotopic Transient Kinetic Analysis (SSITKA) was applied to provide surface residence times and coverages of reaction intermediates as a function of Co particle size (2.6-16 nm). For carbon nanofiber supported cobalt catalysts at 210 degrees C and H(2)/CO = 10 v/v, it appeared that the surface residence times of reversibly bonded CH(x) and OH(x) intermediates increased, whereas that of CO decreased for small (<6 nm) Co particles. A higher coverage of irreversibly bonded CO was found for small Co particles that was ascribed to a larger fraction of low-coordinated surface sites. The coverages and residence times obtained from SSITKA were used to describe the surface-specific activity (TOF) quantitatively and the CH(4) selectivity qualitatively as a function of Co particle size for the FT reaction (220 degrees C, H(2)/CO = 2). The lower TOF of Co particles <6 nm is caused by both blocking of edge/corner sites and a lower intrinsic activity at the small terraces. The higher methane selectivity of small Co particles is mainly brought about by their higher hydrogen coverages.
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Metadata
- Authors
- den Breejen, J. P., Radstake, P. B., Bezemer, G. L., Bitter, J. H., Frøseth, V., Holmen, A., & de Jong, K. P.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2009-04-29
- Volume
- 131
- Issue
- 20
- Pages
- 7197-7203
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2000646281
- Cited by
- 792
- References
- 1
- FWCI
- 10.74
- Type
- journal article
- Language
- en
- Open access
- closed
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