Silver-Promoted Dehydroaromatization of Ethylene over ZSM-5 Catalysts
Abstract
Abstract The shape selectivity of ZSM‐5 (MFI type) catalysts is ideal for the production of C 6 –C 8 aromatics. Developing high‐performance zeolite catalysts with improved selectivity to aromatics, particularly from diversified (non‐petroleum) feedstocks, has broad commercial appeal. Non‐oxidative coupling (NOC) of ethylene was examined over Ag‐ZSM‐5 catalysts at 400 °C and shows that Ag + sites promote dehydroaromatization with enhanced selectivity to toluene and xylenes. Metal exchange of H‐ZSM‐5 results in Ag zoning wherein Ag + site density is higher on the exterior of ZSM‐5 particles. Catalyst performance was characterized with varying Ag loading as well as the use of methane co‐feed. Aromatic selectivity is about 60 % on Ag‐ZSM‐5 compared to 20 % on H‐ZSM‐5, which is qualitatively consistent with density functional theory (DFT) showing that ethylene forms strong complexes with Ag + (Lewis acid) sites. DFT calculations also reveal that ethylene activation on H + (Brønsted acid) sites is more energetically favorable, and likely constitutes the first mechanistic step in ethylene‐to‐liquids (ETL) reactions. Ag‐ZSM‐5 is thus identified as an effective catalyst for low‐temperature ETL reactions that has the potential to outperform conventional metal‐exchanged zeolites.
- Authors:
-
[1];
[1]
- University of Houston, Houston, TX (United States). Dept. of Chemical and Biomolecular Engineering
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1543477
- Alternate Identifier(s):
- OSTI ID: 1401762
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 9; Journal ID: ISSN 1867-3880
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemistry; dehydroaromatization; ethylene upgrading; natural gas; silver; zeolites
Citation Formats
Hsieh, Ming‐Feng, Zhou, Yunwen, Thirumalai, Hari, Grabow, Lars C., and Rimer, Jeffrey D. Silver-Promoted Dehydroaromatization of Ethylene over ZSM-5 Catalysts. United States: N. p., 2017.
Web. doi:10.1002/cctc.201700192.
Hsieh, Ming‐Feng, Zhou, Yunwen, Thirumalai, Hari, Grabow, Lars C., & Rimer, Jeffrey D. Silver-Promoted Dehydroaromatization of Ethylene over ZSM-5 Catalysts. United States. https://doi.org/10.1002/cctc.201700192
Hsieh, Ming‐Feng, Zhou, Yunwen, Thirumalai, Hari, Grabow, Lars C., and Rimer, Jeffrey D. Thu .
"Silver-Promoted Dehydroaromatization of Ethylene over ZSM-5 Catalysts". United States. https://doi.org/10.1002/cctc.201700192. https://www.osti.gov/servlets/purl/1543477.
@article{osti_1543477,
title = {Silver-Promoted Dehydroaromatization of Ethylene over ZSM-5 Catalysts},
author = {Hsieh, Ming‐Feng and Zhou, Yunwen and Thirumalai, Hari and Grabow, Lars C. and Rimer, Jeffrey D.},
abstractNote = {Abstract The shape selectivity of ZSM‐5 (MFI type) catalysts is ideal for the production of C 6 –C 8 aromatics. Developing high‐performance zeolite catalysts with improved selectivity to aromatics, particularly from diversified (non‐petroleum) feedstocks, has broad commercial appeal. Non‐oxidative coupling (NOC) of ethylene was examined over Ag‐ZSM‐5 catalysts at 400 °C and shows that Ag + sites promote dehydroaromatization with enhanced selectivity to toluene and xylenes. Metal exchange of H‐ZSM‐5 results in Ag zoning wherein Ag + site density is higher on the exterior of ZSM‐5 particles. Catalyst performance was characterized with varying Ag loading as well as the use of methane co‐feed. Aromatic selectivity is about 60 % on Ag‐ZSM‐5 compared to 20 % on H‐ZSM‐5, which is qualitatively consistent with density functional theory (DFT) showing that ethylene forms strong complexes with Ag + (Lewis acid) sites. DFT calculations also reveal that ethylene activation on H + (Brønsted acid) sites is more energetically favorable, and likely constitutes the first mechanistic step in ethylene‐to‐liquids (ETL) reactions. Ag‐ZSM‐5 is thus identified as an effective catalyst for low‐temperature ETL reactions that has the potential to outperform conventional metal‐exchanged zeolites.},
doi = {10.1002/cctc.201700192},
journal = {ChemCatChem},
number = 9,
volume = 9,
place = {United States},
year = {Thu Feb 16 00:00:00 EST 2017},
month = {Thu Feb 16 00:00:00 EST 2017}
}
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Figures / Tables:
Figure 1: (A) Powder XRD patterns of (i) H-ZSM-5, (ii) as-prepared Ag25ZSM-5, and (iii) calcined Ag25-ZSM-5 are shown in black, red, and blue, respectively. (B) XPS spectra of (ii) as-prepared Ag25-ZSM-5 and (iii) calcined Ag25-ZSM-5 are shown in red and blue, respectively. Binding energies of 375.3 and 369.3 eV aremore »
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Works referencing / citing this record:
Progress in Developing a Structure‐Activity Relationship for the Direct Aromatization of Methane
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