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Title: The effect of Fe-Rh alloying on CO hydrogenation to C2+ oxygenates

Journal Article · · Journal of Catalysis
 [1];  [1];  [2];  [3];  [4]
  1. Stony Brook Univ., Stony Brook, NY (United States)
  2. Univ. of Catalonia, Barcelona (Spain)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Stony Brook Univ., Stony Brook, NY (United States); Brookhaven National Lab., Upton, NY (United States)
+ Show Author Affiliations

A combination of reactivity and structural studies using X-ray diffraction (XRD), pair distribution function (PDF), and transmission electron microscopy (TEM) was used to identify the active phases of Fe-modified Rh/TiO2 catalysts for the synthesis of ethanol and other C2+ oxygenates from CO hydrogenation. XRD and TEM confirm the existence of Fe–Rh alloys for catalyst with 1–7 wt% Fe and ~2 wt% Rh. Rietveld refinements show that FeRh alloy content increases with Fe loading up to ~4 wt%, beyond which segregation to metallic Fe becomes favored over alloy formation. Catalysts that contain Fe metal after reduction exhibit some carburization as evidenced by the formation of small amounts of Fe3C during CO hydrogenation. Analysis of the total Fe content of the catalysts also suggests the presence of FeOx also increased under reaction conditions. Reactivity studies show that enhancement of ethanol selectivity with Fe loading is accompanied by a significant drop in CO conversion. Comparison of the XRD phase analyses with selectivity suggests that higher ethanol selectivity is correlated with the presence of Fe–Rh alloy phases. As a result, the interface between Fe and Rh serves to enhance the selectivity of ethanol, but suppresses the activity of the catalyst which is attributed to the blocking or modifying of Rh active sites.

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:
1228866
Alternate ID(s):
OSTI ID: 1252810
Report Number(s):
BNL-108607-2015-JA; R&D Project: CO009; KC0302010
Journal Information:
Journal of Catalysis, Vol. 329, Issue C; ISSN 0021-9517
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 37 works
Citation information provided by
Web of Science

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Cited By (6)

Atomic‐Scale Observation of the Metal–Promoter Interaction in Rh‐Based Syngas‐Upgrading Catalysts journal May 2019
Synthesis of higher alcohols by CO hydrogenation on a K-promoted Ni–Mo catalyst derived from Ni–Mo phyllosilicate journal January 2018
Operando monitoring of temperature and active species at the single catalyst particle level journal September 2019
Atomic‐Scale Observation of the Metal–Promoter Interaction in Rh‐Based Syngas‐Upgrading Catalysts journal June 2019
Status and prospects in higher alcohols synthesis from syngas journal January 2017
Synergetic catalysis of bimetallic copper–cobalt nanosheets for direct synthesis of ethanol and higher alcohols from syngas journal January 2018

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
ethanol synthesis
bimetallic catalysts
CO hydrogenation