Deactivation by Potassium Accumulation on a Pt/TiO2 Bifunctional Catalyst for Biomass Catalytic Fast Pyrolysis

Lin, Fan; Lu, Yubing; Unocic, Kinga A.; Habas, Susan E.; Griffin, Michael B.; Schaidle, Joshua A.; Meyer, Harry M.; Wang, Yong; Wang, Huamin

doi:10.1021/acscatal.1c02368

Title: Deactivation by Potassium Accumulation on a Pt/TiO₂ Bifunctional Catalyst for Biomass Catalytic Fast Pyrolysis

Journal Article · 16 December 2021 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.1c02368 · OSTI ID:1841144

Lin, Fan ^[1]; Lu, Yubing ^[1]; Unocic, Kinga A. ^[2];

^[3]; Griffin, Michael B. ^[3];

^[3]; Meyer, Harry M. ^[2];

^[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)

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.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Bioenergy Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; AC05-76RL01830; AC36-08GO28308

OSTI ID:: 1841144

Report Number(s):: NREL/JA-5100-80303; PNNL-SA-168817; MainId:42506; UUID:500b473d-f5af-402b-b7b3-ee29ae4d2b75; MainAdminID:63644

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 1 Vol. 12; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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09 BIOMASS FUELS
Pt/TiO2
biomass
catalytic fast pyrolysis
deactivation
potassium

Title: Deactivation by Potassium Accumulation on a Pt/TiO2 Bifunctional Catalyst for Biomass Catalytic Fast Pyrolysis

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Title: Deactivation by Potassium Accumulation on a Pt/TiO₂ Bifunctional Catalyst for Biomass Catalytic Fast Pyrolysis