Fischer-Tropsch Synthesis: XANES Investigation of Hydrogen Chloride Poisoned Iron and Cobalt-Based Catalysts at the K-Edges of Cl, Fe, and Co

Pendyala, Venkat Ramana Rao; Jacobs, Gary; Ma, Wenping; Sparks, Dennis E.; Shafer, Wilson D.; Khalid, Syed; Xiao, Qunfeng; Hu, Yongfeng; Davis, Burtron H.

doi:10.1007/s10562-016-1820-8

Title: Fischer-Tropsch Synthesis: XANES Investigation of Hydrogen Chloride Poisoned Iron and Cobalt-Based Catalysts at the K-Edges of Cl, Fe, and Co

Journal Article · Sat Jul 23 00:00:00 EDT 2016 · Catalysis Letters

DOI:https://doi.org/10.1007/s10562-016-1820-8· OSTI ID:1340425

Pendyala, Venkat Ramana Rao ^[1]; Jacobs, Gary ^[1]; Ma, Wenping ^[1]; Sparks, Dennis E. ^[1]; Shafer, Wilson D. ^[1]; Khalid, Syed ^[2]; Xiao, Qunfeng ^[3]; Hu, Yongfeng ^[3]; Davis, Burtron H. ^[1]

Univ. of Kentucky, Lexington, KY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Canadian Light Sources, Inc., Saskatoon, SK (Canada)

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 [ACS Catal. 5 (2015) 3124-3136 and DOE final report 2011; Catal. Lett. 144 (2014) 1127-1133]. 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 HCl poisoning mechanism on the iron and cobalt catalysts. Cl K-edge normalized XANES results 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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC00112704

OSTI ID:: 1340425

Report Number(s):: BNL-113340-2016-JA

Journal Information:: Catalysis Letters, Vol. 146, Issue 10; ISSN 1011-372X

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 10 works

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Related Subjects

10 SYNTHETIC FUELS
Fischer-Tropsch synthesis
iron
cobalt
hydrogen chloride
activity
selectivity
XANES

Title: Fischer-Tropsch Synthesis: XANES Investigation of Hydrogen Chloride Poisoned Iron and Cobalt-Based Catalysts at the K-Edges of Cl, Fe, and Co

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