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:
-
[1];
[2];
[3];
[1];
[3];
[3];
[1];
[1]
- Georgia Institute of Technology, Atlanta, GA (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- 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. doi: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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