Deactivation by Potassium Accumulation on a Pt/TiO2 Bifunctional Catalyst for Biomass Catalytic Fast Pyrolysis
Abstract
Biomass-derived feedstocks bring significant challenges to the longevity of the catalysts used for their conversion, and alkali metals, for example, K, in the feedstock have been widely ascribed as one of the important factors causing catalyst deactivation. To address this challenge, it is critical to understand the mechanism of catalyst deactivation caused by K accumulation to guide the improvement of catalysts and processes and the development of catalyst regeneration strategies. In this work, we report a deep understanding of the impact of K on a bifunctional Pt/TiO2 catalyst, which is an efficient catalyst for the ex situ catalytic fast pyrolysis of biomass. We simulated the K-poisoning of Pt/TiO2 catalysts by purposely loading different amounts of K (100-6000 ppm by weight) on the catalysts. A series of characterization approaches, including scanning transmission electron microscopy, Fourier transform infrared spectroscopy, and chemical titration, were combined with a kinetic assessment of multiple probe reactions to elucidate the mechanism of Pt/TiO2 deactivation by K accumulation. At low K loadings (<800 ppm), K preferentially poisons the strong Lewis acid sites, leading to significantly reduced activity for acid-catalyzed alcohol dehydration. However, acetone condensation is less sensitive to the poisoning of strong Lewis acid sites. Reactions that occurmore »
- Authors:
-
[3];
[3];
[4];
[1]
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Bioenergy Technologies Office
- OSTI Identifier:
- 1841144
- Alternate Identifier(s):
- OSTI ID: 1854849
- Report Number(s):
- NREL/JA-5100-80303; PNNL-SA-168817
Journal ID: ISSN 2155-5435; MainId:42506;UUID:500b473d-f5af-402b-b7b3-ee29ae4d2b75;MainAdminID:63644
- Grant/Contract Number:
- AC36-08GO28308; AC05- 00OR22725; AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 1; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 09 BIOMASS FUELS; biomass; catalytic fast pyrolysis; deactivation; potassium; Pt/TiO2
Citation Formats
Lin, Fan, Lu, Yubing, Unocic, Kinga A., Habas, Susan E., Griffin, Michael B., Schaidle, Joshua A., Meyer, Harry M., Wang, Yong, and Wang, Huamin. Deactivation by Potassium Accumulation on a Pt/TiO2 Bifunctional Catalyst for Biomass Catalytic Fast Pyrolysis. United States: N. p., 2021.
Web. doi:10.1021/acscatal.1c02368.
Lin, Fan, Lu, Yubing, Unocic, Kinga A., Habas, Susan E., Griffin, Michael B., Schaidle, Joshua A., Meyer, Harry M., Wang, Yong, & Wang, Huamin. Deactivation by Potassium Accumulation on a Pt/TiO2 Bifunctional Catalyst for Biomass Catalytic Fast Pyrolysis. United States. https://doi.org/10.1021/acscatal.1c02368
Lin, Fan, Lu, Yubing, Unocic, Kinga A., Habas, Susan E., Griffin, Michael B., Schaidle, Joshua A., Meyer, Harry M., Wang, Yong, and Wang, Huamin. Fri .
"Deactivation by Potassium Accumulation on a Pt/TiO2 Bifunctional Catalyst for Biomass Catalytic Fast Pyrolysis". United States. https://doi.org/10.1021/acscatal.1c02368. https://www.osti.gov/servlets/purl/1841144.
@article{osti_1841144,
title = {Deactivation by Potassium Accumulation on a Pt/TiO2 Bifunctional Catalyst for Biomass Catalytic Fast Pyrolysis},
author = {Lin, Fan and Lu, Yubing and Unocic, Kinga A. and Habas, Susan E. and Griffin, Michael B. and Schaidle, Joshua A. and Meyer, Harry M. and Wang, Yong and Wang, Huamin},
abstractNote = {Biomass-derived feedstocks bring significant challenges to the longevity of the catalysts used for their conversion, and alkali metals, for example, K, in the feedstock have been widely ascribed as one of the important factors causing catalyst deactivation. To address this challenge, it is critical to understand the mechanism of catalyst deactivation caused by K accumulation to guide the improvement of catalysts and processes and the development of catalyst regeneration strategies. In this work, we report a deep understanding of the impact of K on a bifunctional Pt/TiO2 catalyst, which is an efficient catalyst for the ex situ catalytic fast pyrolysis of biomass. We simulated the K-poisoning of Pt/TiO2 catalysts by purposely loading different amounts of K (100-6000 ppm by weight) on the catalysts. A series of characterization approaches, including scanning transmission electron microscopy, Fourier transform infrared spectroscopy, and chemical titration, were combined with a kinetic assessment of multiple probe reactions to elucidate the mechanism of Pt/TiO2 deactivation by K accumulation. At low K loadings (<800 ppm), K preferentially poisons the strong Lewis acid sites, leading to significantly reduced activity for acid-catalyzed alcohol dehydration. However, acetone condensation is less sensitive to the poisoning of strong Lewis acid sites. Reactions that occur on Pt sites or at the metal-support interface, including alkene hydrogenation, m-cresol hydrodeoxygenation (HDO), and CO oxidation, were not impacted. At high K loadings (>800 ppm), K starts to accumulate on the Pt-TiO2 interfacial area, poisoning the interfacial active sites for HDO and CO oxidation reactions. We further found that the poisoning of the Pt/TiO2 catalyst by K is reversible, and water washing can successfully remove the accumulated K and recover the activities for both alcohol dehydration and m-cresol HDO reactions.},
doi = {10.1021/acscatal.1c02368},
journal = {ACS Catalysis},
number = 1,
volume = 12,
place = {United States},
year = {Fri Dec 17 00:00:00 EST 2021},
month = {Fri Dec 17 00:00:00 EST 2021}
}
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