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Title: In-situ IR Spectroscopy Study of Reactions of C3 Oxygenates on Heteroatom (Sn, Mo, and W) doped BEA Zeolites and the Effect of Co-adsorbed Water

Abstract

The reactions of acetone and hydroxyacetone over heteroatom doped BEA zeolites (Sn, Mo, and W) in the presence and absence of H2O vapor are investigated using infrared spectroscopy. Acetone is converted to mesityl oxide over Sn-BEA exclusively. At higher temperatures, larger oxygenates such as phorones, aromatics, and coke form. The presence of co-adsorbed water in Sn-BEA suppresses tautomerization. H2O vapor is also beneficial for minimizing coke formation at high temperatures. Hydroxyacetone is converted into 2-hydroxypropanal over Sn-BEA, exhibiting high affinity to Sn sites up to 400 °C. Sn-BEA catalyzes conversion of hydroxyacetone into the enol in the absence of H2O, but exposure to H2O induces the formation of 2-hydroxypropanal and subsequent conversion to acrolein. Furthermore, the Lewis acid descriptors are used to rationalize the reaction pathways. For the isomerization of hydroxyacetone into 2-hydroxypropanal, the hardness of acid sites influences the reaction and correlates with the overall Lewis acidity of the catalysts, respectively. However, the size of the exchanged metal significantly affects aldol condensation, where keto and enol forms of acetone adsorb to active sites simultaneously.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]
  1. Georgia Institute of Technology, Atlanta, GA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  3. Univ. of Wisconsin, Madison, WI (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1737430
Report Number(s):
BNL-220718-2020-JAAM
Journal ID: ISSN 1867-3880
Grant/Contract Number:  
SC0012704; CBET-1705444; DGE-1650044; SC0016486
Resource Type:
Accepted Manuscript
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Volume: 13; Journal Issue: 1; Journal ID: ISSN 1867-3880
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Biomass; isomerization; C-C coupling; deactivation; Lewis acid site

Citation Formats

Najmi, Sean, So, Jungseob, Stavitski, Eli, McDermott, William P., Lyu, Yimeng, Burt, Sam P., Hermans, Ive, Sholl, David S., and Sievers, Carsten. In-situ IR Spectroscopy Study of Reactions of C3 Oxygenates on Heteroatom (Sn, Mo, and W) doped BEA Zeolites and the Effect of Co-adsorbed Water. United States: N. p., 2020. Web. https://doi.org/10.1002/cctc.202001424.
Najmi, Sean, So, Jungseob, Stavitski, Eli, McDermott, William P., Lyu, Yimeng, Burt, Sam P., Hermans, Ive, Sholl, David S., & Sievers, Carsten. In-situ IR Spectroscopy Study of Reactions of C3 Oxygenates on Heteroatom (Sn, Mo, and W) doped BEA Zeolites and the Effect of Co-adsorbed Water. United States. https://doi.org/10.1002/cctc.202001424
Najmi, Sean, So, Jungseob, Stavitski, Eli, McDermott, William P., Lyu, Yimeng, Burt, Sam P., Hermans, Ive, Sholl, David S., and Sievers, Carsten. Wed . "In-situ IR Spectroscopy Study of Reactions of C3 Oxygenates on Heteroatom (Sn, Mo, and W) doped BEA Zeolites and the Effect of Co-adsorbed Water". United States. https://doi.org/10.1002/cctc.202001424. https://www.osti.gov/servlets/purl/1737430.
@article{osti_1737430,
title = {In-situ IR Spectroscopy Study of Reactions of C3 Oxygenates on Heteroatom (Sn, Mo, and W) doped BEA Zeolites and the Effect of Co-adsorbed Water},
author = {Najmi, Sean and So, Jungseob and Stavitski, Eli and McDermott, William P. and Lyu, Yimeng and Burt, Sam P. and Hermans, Ive and Sholl, David S. and Sievers, Carsten},
abstractNote = {The reactions of acetone and hydroxyacetone over heteroatom doped BEA zeolites (Sn, Mo, and W) in the presence and absence of H2O vapor are investigated using infrared spectroscopy. Acetone is converted to mesityl oxide over Sn-BEA exclusively. At higher temperatures, larger oxygenates such as phorones, aromatics, and coke form. The presence of co-adsorbed water in Sn-BEA suppresses tautomerization. H2O vapor is also beneficial for minimizing coke formation at high temperatures. Hydroxyacetone is converted into 2-hydroxypropanal over Sn-BEA, exhibiting high affinity to Sn sites up to 400 °C. Sn-BEA catalyzes conversion of hydroxyacetone into the enol in the absence of H2O, but exposure to H2O induces the formation of 2-hydroxypropanal and subsequent conversion to acrolein. Furthermore, the Lewis acid descriptors are used to rationalize the reaction pathways. For the isomerization of hydroxyacetone into 2-hydroxypropanal, the hardness of acid sites influences the reaction and correlates with the overall Lewis acidity of the catalysts, respectively. However, the size of the exchanged metal significantly affects aldol condensation, where keto and enol forms of acetone adsorb to active sites simultaneously.},
doi = {10.1002/cctc.202001424},
journal = {ChemCatChem},
number = 1,
volume = 13,
place = {United States},
year = {2020},
month = {11}
}

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Identification of molybdenum oxide nanostructures on zeolites for natural gas conversion
journal, April 2015


Activation of Mo and V oxides supported on ZSM-5 zeolite catalysts followed by in situ XAS and XRD and their uses in oxydehydration of glycerol
journal, February 2020


Toward Functional Polyester Building Blocks from Renewable Glycolaldehyde with Sn Cascade Catalysis
journal, July 2013

  • Dusselier, Michiel; Van Wouwe, Pieter; De Smet, Sanne
  • ACS Catalysis, Vol. 3, Issue 8
  • DOI: 10.1021/cs400298n

Synthesis of Itaconic Acid Ester Analogues via Self-Aldol Condensation of Ethyl Pyruvate Catalyzed by Hafnium BEA Zeolites
journal, April 2016


Preparation and characterization of WOx/ZrO2 nanosized catalysts with high WOx dispersion threshold and acidity
journal, March 2013


Role of silanol groups in the incorporation of V in β zeolite
journal, April 2000

  • Dzwigaj, Stanislaw; Massiani, Pascale; Davidson, Anne
  • Journal of Molecular Catalysis A: Chemical, Vol. 155, Issue 1-2
  • DOI: 10.1016/S1381-1169(99)00332-5

Exploring the multifunctionality and accessibility of vanadosilicates to produce acrylic acid in one-pot glycerol oxydehydration
journal, July 2020

  • Vieira, Luiz H.; Lopez-Castillo, Alejandro; Jones, Christopher W.
  • Applied Catalysis A: General, Vol. 602
  • DOI: 10.1016/j.apcata.2020.117687