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Title: Driving towards cost-competitive biofuels through catalytic fast pyrolysis by rethinking catalyst selection and reactor configuration

Catalytic fast pyrolysis (CFP) has emerged as an attractive process for the conversion of lignocellulosic biomass into renewable fuels and products. Considerable research and development has focused on using circulating-bed reactors with zeolite catalysts (e.g., HZSM-5) for CFP because of their propensity to form gasoline-range aromatic hydrocarbons. However, the high selectivity for aromatics comes at the expense of low carbon yield, a key economic driver for this process. In this contribution, we evaluate non-zeolite catalysts in a fixed-bed reactor configuration for an integrated CFP process to produce fuel blendstocks from lignocellulosic biomass. These experimental efforts are coupled with technoeconomic analysis (TEA) to benchmark the process and guide research and development activities to minimize costs. The results indicate that CFP bio-oil can be produced from pine with improved yield by using a bifunctional metal-acid 2 wt% Pt/TiO 2 catalyst in a fixed-bed reactor operated with co-fed H 2 at near atmospheric pressure, as compared to H-ZSM5 in a circulating-bed reactor. The Pt/TiO 2 catalyst exhibited good stability over 13 reaction-regeneration cycles with no evidence of irreversible deactivation. The CFP bio-oil was continuously hydrotreated for 140 h time-on-stream using a single-stage system with 84 wt% of the hydrotreated product having a boilingmore » point in the gasoline and distillate range. This integrated biomass-to-blendstock process was determined to exhibit an energy efficiency of 50% and a carbon efficiency of 38%, based on the experimental results and process modelling. TEA of the integrated process revealed a modelled minimum fuel selling price (MFSP) of $4.34 per gasoline gallon equivalent (GGE), which represents a cost reduction of $0.85 GGE -1 compared to values reported for CFP with a zeolite catalyst. TEA also indicated that catalyst cost was a significant factor influencing the MFSP, which informed additional CFP experiments in which lower-cost Mo2C and high-dispersion 0.5 wt% Pt/TiO 2 catalysts were synthesized and evaluated. These materials demonstrated CFP carbon yield and oil oxygen content similar to those of the 2 wt% Pt/TiO 2 catalyst, offering proof-of-concept that the lower-cost catalysts can be effective for CFP and providing a route to reduce the modelled MFSP to $3.86–3.91 GGE -1. This report links foundational science and applied engineering to demonstrate the potential of fixed-bed CFP and highlights the impact of coupled TEA to guide research activities towards cost reductions.« less
Authors:
ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [3] ; ORCiD logo [1] ; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Report Number(s):
NREL/JA-5100-71877
Journal ID: ISSN 1754-5692; EESNBY
Grant/Contract Number:
AC36-08GO28308; AC02-06CH-11357; AC06-76RLO-1830; AC36-08-GO28308
Type:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Name: Energy & Environmental Science; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B)
Country of Publication:
United States
Language:
English
Subject:
09 BIOMASS FUELS; catalytic fast pyrolysis; biomass; bio-oil
OSTI Identifier:
1468521
Alternate Identifier(s):
OSTI ID: 1465598

Griffin, Michael B., Iisa, Kristiina, Wang, Huamin, Dutta, Abhijit, Orton, Kellene A., French, Richard J., Santosa, Daniel M., Wilson, Nolan, Christensen, Earl, Nash, Connor, Van Allsburg, Kurt M., Baddour, Frederick G., Ruddy, Daniel A., Tan, Eric C. D., Cai, Hao, Mukarakate, Calvin, and Schaidle, Joshua A.. Driving towards cost-competitive biofuels through catalytic fast pyrolysis by rethinking catalyst selection and reactor configuration. United States: N. p., Web. doi:10.1039/C8EE01872C.
Griffin, Michael B., Iisa, Kristiina, Wang, Huamin, Dutta, Abhijit, Orton, Kellene A., French, Richard J., Santosa, Daniel M., Wilson, Nolan, Christensen, Earl, Nash, Connor, Van Allsburg, Kurt M., Baddour, Frederick G., Ruddy, Daniel A., Tan, Eric C. D., Cai, Hao, Mukarakate, Calvin, & Schaidle, Joshua A.. Driving towards cost-competitive biofuels through catalytic fast pyrolysis by rethinking catalyst selection and reactor configuration. United States. doi:10.1039/C8EE01872C.
Griffin, Michael B., Iisa, Kristiina, Wang, Huamin, Dutta, Abhijit, Orton, Kellene A., French, Richard J., Santosa, Daniel M., Wilson, Nolan, Christensen, Earl, Nash, Connor, Van Allsburg, Kurt M., Baddour, Frederick G., Ruddy, Daniel A., Tan, Eric C. D., Cai, Hao, Mukarakate, Calvin, and Schaidle, Joshua A.. 2018. "Driving towards cost-competitive biofuels through catalytic fast pyrolysis by rethinking catalyst selection and reactor configuration". United States. doi:10.1039/C8EE01872C.
@article{osti_1468521,
title = {Driving towards cost-competitive biofuels through catalytic fast pyrolysis by rethinking catalyst selection and reactor configuration},
author = {Griffin, Michael B. and Iisa, Kristiina and Wang, Huamin and Dutta, Abhijit and Orton, Kellene A. and French, Richard J. and Santosa, Daniel M. and Wilson, Nolan and Christensen, Earl and Nash, Connor and Van Allsburg, Kurt M. and Baddour, Frederick G. and Ruddy, Daniel A. and Tan, Eric C. D. and Cai, Hao and Mukarakate, Calvin and Schaidle, Joshua A.},
abstractNote = {Catalytic fast pyrolysis (CFP) has emerged as an attractive process for the conversion of lignocellulosic biomass into renewable fuels and products. Considerable research and development has focused on using circulating-bed reactors with zeolite catalysts (e.g., HZSM-5) for CFP because of their propensity to form gasoline-range aromatic hydrocarbons. However, the high selectivity for aromatics comes at the expense of low carbon yield, a key economic driver for this process. In this contribution, we evaluate non-zeolite catalysts in a fixed-bed reactor configuration for an integrated CFP process to produce fuel blendstocks from lignocellulosic biomass. These experimental efforts are coupled with technoeconomic analysis (TEA) to benchmark the process and guide research and development activities to minimize costs. The results indicate that CFP bio-oil can be produced from pine with improved yield by using a bifunctional metal-acid 2 wt% Pt/TiO2 catalyst in a fixed-bed reactor operated with co-fed H2 at near atmospheric pressure, as compared to H-ZSM5 in a circulating-bed reactor. The Pt/TiO2 catalyst exhibited good stability over 13 reaction-regeneration cycles with no evidence of irreversible deactivation. The CFP bio-oil was continuously hydrotreated for 140 h time-on-stream using a single-stage system with 84 wt% of the hydrotreated product having a boiling point in the gasoline and distillate range. This integrated biomass-to-blendstock process was determined to exhibit an energy efficiency of 50% and a carbon efficiency of 38%, based on the experimental results and process modelling. TEA of the integrated process revealed a modelled minimum fuel selling price (MFSP) of $4.34 per gasoline gallon equivalent (GGE), which represents a cost reduction of $0.85 GGE-1 compared to values reported for CFP with a zeolite catalyst. TEA also indicated that catalyst cost was a significant factor influencing the MFSP, which informed additional CFP experiments in which lower-cost Mo2C and high-dispersion 0.5 wt% Pt/TiO2 catalysts were synthesized and evaluated. These materials demonstrated CFP carbon yield and oil oxygen content similar to those of the 2 wt% Pt/TiO2 catalyst, offering proof-of-concept that the lower-cost catalysts can be effective for CFP and providing a route to reduce the modelled MFSP to $3.86–3.91 GGE-1. This report links foundational science and applied engineering to demonstrate the potential of fixed-bed CFP and highlights the impact of coupled TEA to guide research activities towards cost reductions.},
doi = {10.1039/C8EE01872C},
journal = {Energy & Environmental Science},
number = ,
volume = ,
place = {United States},
year = {2018},
month = {8}
}

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