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- Title
Fischer-Tropsch Synthesis: XANES Investigation of Hydrogen Chloride Poisoned Iron and Cobalt-Based Catalysts at the K-Edges of Cl, Fe, and Co.
- Authors
Pendyala, Venkat; Jacobs, Gary; Ma, Wenping; Sparks, Dennis; Shafer, Wilson; Khalid, Syed; Xiao, Qunfeng; Hu, Yongfeng; Davis, Burtron
- Abstract
The effect of co-fed hydrogen chloride (HCl) in syngas on the performance of iron and cobalt-based Fischer-Tropsch (FT) catalysts was investigated in our earlier studies (Ma et al. in ACS Catal 5:3124-3136, 2015; Davis et al., DOE final report, 2011; Gnanamani et al. in Catal Lett 144:1127-1133, 2014). For an iron catalyst, lower HCl concentrations (<2.0 ppmw of HCl)) in syngas did not significantly affect the activity, whereas rapid deactivation occurred at higher concentrations (~20 ppmw). With cobalt catalysts, even low concentrations of HCl (100 ppbw) caused catalyst deactivation, and the deactivation rate increased with increasing HCl concentration in the syngas. The deactivation of the catalysts is explained by the chloride being adsorbed on the catalyst surface to (1) block the active sites and/or (2) electronically modify the sites. In this study, XANES spectroscopy was employed to investigate the HCl poisoning mechanism on the iron and cobalt catalysts. Normalized XANES spectra recorded at the Cl K-edge indicate that Cl is indeed present on the catalyst following HCl poisoning and exhibits a structure similar to the family of compounds MCl; two main peaks are formed, with the second peak consisting of a main peak and a higher energy shoulder. At the Co K and Fe K edges, the white line was observed to be slightly increased relative to the same catalyst under clean conditions. There is then the additional possibility that Cl adsorption may act in part to intercept electron density from the FT metallic function (e.g., cobalt or iron carbide). If so, this would result in less back-donation and therefore hinder the scission of molecules such as CO. Graphical Abstract:
- Subjects
FISCHER-Tropsch process; HYDROGEN chloride; COBALT catalysts; IRON catalysts; SYNTHESIS gas
- Publication
Catalysis Letters, 2016, Vol 146, Issue 10, p1858
- ISSN
1011-372X
- Publication type
Article
- DOI
10.1007/s10562-016-1820-8