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Title: In Situ Formation of FeRh Nanoalloys for Oxygenate Synthesis

Abstract

Early and late transition metals are often combined as a strategy to tune the selectivity of catalysts for the conversion of syngas (CO/H2) to C2+ oxygenates, such as ethanol. Here we show how the use of a highly reducible Fe2O3 support for Rh leads to the in situ formation of supported FeRh nanoalloy catalysts that exhibit high selectivity for ethanol synthesis. In situ characterizations by X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS) reveal the coexistence of iron oxide, iron carbide, metallic iron, and FeRh alloy phases depending on reaction conditions and Rh loading. Structural analysis coupled with catalytic testing indicates that oxygenate formation is correlated to the presence of FeRh alloys, while the iron oxide and carbide phases lead mainly to hydrocarbons. Finally, the formation of nanoalloys by in situ reduction of a metal oxide support under working conditions represents a simple approach for the preparation bimetallic catalysts with enhanced catalytic properties.

Authors:
 [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [3]
  1. Stony Brook Univ., NY (United States). Dept. of Chemistry
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division; Stony Brook Univ., NY (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1462400
Report Number(s):
BNL-207863-2018-JAAM
Journal ID: ISSN 2155-5435
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CO hydrogenation; heterogeneous catalysis; in situ characterization; iron−rhodium alloy; oxygenate synthesis; supported catalysts

Citation Formats

Carrillo, Pamela, Shi, Rui, Teeluck, Krishani, Senanayake, Sanjaya D., and White, Michael G. In Situ Formation of FeRh Nanoalloys for Oxygenate Synthesis. United States: N. p., 2018. Web. doi:10.1021/acscatal.8b02235.
Carrillo, Pamela, Shi, Rui, Teeluck, Krishani, Senanayake, Sanjaya D., & White, Michael G. In Situ Formation of FeRh Nanoalloys for Oxygenate Synthesis. United States. https://doi.org/10.1021/acscatal.8b02235
Carrillo, Pamela, Shi, Rui, Teeluck, Krishani, Senanayake, Sanjaya D., and White, Michael G. Wed . "In Situ Formation of FeRh Nanoalloys for Oxygenate Synthesis". United States. https://doi.org/10.1021/acscatal.8b02235. https://www.osti.gov/servlets/purl/1462400.
@article{osti_1462400,
title = {In Situ Formation of FeRh Nanoalloys for Oxygenate Synthesis},
author = {Carrillo, Pamela and Shi, Rui and Teeluck, Krishani and Senanayake, Sanjaya D. and White, Michael G.},
abstractNote = {Early and late transition metals are often combined as a strategy to tune the selectivity of catalysts for the conversion of syngas (CO/H2) to C2+ oxygenates, such as ethanol. Here we show how the use of a highly reducible Fe2O3 support for Rh leads to the in situ formation of supported FeRh nanoalloy catalysts that exhibit high selectivity for ethanol synthesis. In situ characterizations by X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS) reveal the coexistence of iron oxide, iron carbide, metallic iron, and FeRh alloy phases depending on reaction conditions and Rh loading. Structural analysis coupled with catalytic testing indicates that oxygenate formation is correlated to the presence of FeRh alloys, while the iron oxide and carbide phases lead mainly to hydrocarbons. Finally, the formation of nanoalloys by in situ reduction of a metal oxide support under working conditions represents a simple approach for the preparation bimetallic catalysts with enhanced catalytic properties.},
doi = {10.1021/acscatal.8b02235},
journal = {ACS Catalysis},
number = ,
volume = 8,
place = {United States},
year = {Wed Jun 27 00:00:00 EDT 2018},
month = {Wed Jun 27 00:00:00 EDT 2018}
}

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Works referencing / citing this record:

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