Abstract
Chemical reaction kinetics enable predictive scaling studies and process sensitivity analyses that can substantially accelerate commercial deployment of new catalytic transformation technologies. The absence of suitable kinetic parameters for catalytic fast pyrolysis (CFP) of biomass feedstocks has precluded such de-risking simulation activities. In this work we consider ex situ CFP using a Pt/TiO2 catalyst in a packed bed vapor phase upgrading reactor (VPU) with co-fed H2. We develop a multiscale simulation framework to de-couple apparent kinetics from both intraparticle and reactor-scale transport phenomena. The transport model is integrated with a kinetic scheme that predicts (1) lumped yields of product partially deoxygenated compounds, hydrocarbons, light gases, water, and coke, as well as (2) active site concentration and deactivation of the catalyst. We employ recent advancements in mathematical treatments of cascading reaction systems in the context of an axial-dispersion packed bed reactor model to achieve a rapidly-solving simulation framework that is amenable to iterative regression for kinetic parameter extraction. Results demonstrate accurate predictions of CFP yields within 5% for a variety of conditions, including different reaction times, Pt loadings, and variations in feedstock attributes.
| Original language | English |
|---|---|
| Pages (from-to) | 125-137 |
| Number of pages | 13 |
| Journal | Reaction Chemistry and Engineering |
| Volume | 6 |
| Issue number | 1 |
| DOIs | |
| State | Published - Jan 2021 |
Funding
This work was authored by the National Renewable Energy Laboratory, operated by Alliance for Sustainable Energy, LLC, for the U.S. Department of Energy (DOE) under Contract No. DE-AC36-08GO28308. Funding provided by U.S. Department of Energy Office of Energy Efficiency and Renewable Energy Solar Energy Technologies Office and in collaboration with the Chemical Catalysis for Bioenergy Consortium (ChemCatBio), a member of the Energy Materials Network (EMN). The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U. S. Government purposes. Scott Palmer, Kellene Orton, Chris Golubieski, Rebecca Jackson, Kathleen Brown, and Earl Christensen are acknowledged for their contributions in performing the experiments and analyzing the data. Aaron Lattanzi is acknowledged for his helpful discussions regarding the packed bed reactor model with MEV. The authors would also like to thank Michael Watson and Luke Tuxworth of Johnson Matthey for their important contributions to this work.
| Funders | Funder number |
|---|---|
| U.S. Department of Energy | DE-AC36-08GO28308 |
