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5. From Biomass to Fuel Blendstocks via Catalytic Fast Pyrolysis and Hydrotreating: An Evaluation of Carbon Efficiency and Fuel Properties for Three Pathways

Author

Iisa, Kristiina, primary, Mukarakate, Calvin, additional, French, Richard J., additional, Agblevor, Foster A., additional, Santosa, Daniel M., additional, Wang, Huamin, additional, Wilson, A. Nolan, additional, Christensen, Earl, additional, Griffin, Michael B., additional, and Schaidle, Joshua A., additional

Published
2023
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7. Enhanced Catalyst Durability for Bio-Based Adipic Acid Production by Atomic Layer Deposition

Author

Settle, Amy E., Cleveland, Nicholas S., Farberow, Carrie A., Conklin, Davis R., Huo, Xiangchen, Dameron, Arrelaine A., Tracy, Ryon W., Sarkar, Reuben, Kautz, Elizabeth J., Devaraj, Arun, Ramasamy, Karthikeyan K., Watson, Mike J., York, Allyson M., Richards, Ryan M., Unocic, Kinga A., Beckham, Gregg T., Griffin, Michael B., Hurst, Katherine E., Tan, Eric C.D., Christensen, Steven T., and Vardon, Derek R.

Published
2019
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11. Advancements and challenges in the production of low-carbon fuels via catalytic fast pyrolysis of biomass through refinery integration and co-product generation.

Author

Yung, Matthew M., Mukarakate, Calvin, Iisa, Kristiina, Wilson, A. Nolan, Nimlos, Mark R., Habas, Susan E., Dutta, Abhijit, Unocic, Kinga A., Schaidle, Joshua A., and Griffin, Michael B.

Subjects
GREENHOUSE gas mitigation, BIOMASS, CETANE number, CHEMICAL transportation, CATALYST poisoning, FOSSIL fuels
Abstract

The production of advanced biofuels represents a near-term opportunity to decarbonize the heavy vehicle transportation sector. However, important barriers must be overcome and successful deployment of these technologies will require (i) catalyst and process development to reduce cost and improve carbon utilization and (ii) industry-relevant validation of operability to de-risk scale-up. Herein, we seek to address these challenges for an integrated two-step process involving catalytic fast pyrolysis (CFP) followed by co-hydrotreating of bio-oil with refinery streams. Technoeconomic and lifecycle analysis based on the data presented herein reveal the potential to generate low-carbon transportation fuels and chemical co-products with a modelled selling price of $2.83 gasoline gallon equivalent (2016$) and a 78% reduction in greenhouse gas emissions compared to fossil-based pathways. The feedstock for this research was a blend of 50 wt% loblolly pine and 50 wt% waste forest residues, and the CFP step was performed using an ex situ fixed bed of Pt/TiO2 with co-fed H2 at atmospheric pressure. Compared to previous state-of-technology benchmarks, advancements in catalyst design and synthesis methodology enabled a four-fold reduction in Pt loading and a 400% increase in time on stream without negatively impacting upgrading performance. Additionally, a first-of-its-kind integrated assessment of waste gas adsorption showed near quantitative recovery of acetone and 2-butanone, which collectively represent approximately 5% of the biomass carbon. The valorization of these co-products opens opportunities to support decarbonization of the chemical sector while simultaneously improving the overall process carbon efficiency to >40%. After condensation, the CFP-oil was co-hydrotreated with straight run diesel (10 : 90 vol%) to achieve 95% biogenic carbon incorporation. The oxygen content of the hydrotreated oil was below detection limits, and the diesel fraction exhibited a cetane number and cloud point suitable for a finished fuel. This manuscript concludes by highlighting remaining research needs associated with improving thermal management during catalyst regeneration, mitigating catalyst deactivation due to inorganic deposition, and demonstrating the durability of biomass feeding systems when operated in hydrogen-rich environments. [ABSTRACT FROM AUTHOR]

Published
2023
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12. Compositional dependence of hydrodeoxygenation pathway selectivity for Ni2−xRhxP nanoparticle catalysts.

Author

LiBretto, Nicole J., Tacey, Sean A., Zubair, Muhammad, Bui, Tuong V., Unocic, Kinga A., Baddour, Frederick G., Griffin, Michael B., Schaidle, Joshua A., Farberow, Carrie A., Ruddy, Daniel A., Bedford, Nicholas M., and Habas, Susan E.

Abstract

Transition-metal phosphides (TMPs) are promising materials for biomass conversion processes, where their metal–acid bifunctionality provides active sites for the necessary variety of catalytic reactions (e.g., hydrogenation, hydrogenolysis, decarbonylation, and dehydration). Aiming to understand the catalytic performance of ternary TMP catalysts for the hydrodeoxygenation (HDO) reaction of biomass-derived oxygenates, a synthetic protocol was developed herein to prepare a series of ternary Ni2−xRhxP nanoparticles (NPs), incorporating Rh into a parent Ni2P template. This solution synthesis method allowed for a series of NPs to be prepared having precisely controlled compositions with similar morphology and crystalline structure. Detailed characterization of this series of Ni2−xRhxP (x ≤ 1) NPs revealed that Rh substituted into the parent hexagonal crystal lattice of Ni2P with concomitant expansion of the lattice. The influence of composition on the catalytic performance of silica-supported Ni2−xRhxP (x = 0 to 0.8, and cubic Rh2P) NPs was investigated through the HDO reaction of m-cresol. Whereas Rh2P was more selective for direct deoxygenation relative to Ni2P, increasing concentrations of Rh in Ni2−xRhxP resulted in a decreased selectivity to direct deoxygenation products (i.e., toluene, benzene, xylene), and an associated increased selectivity to hydrogenation products (i.e., methylcyclohexene). Through in situ high energy X-ray diffraction and density functional theory modeling, we identified OH* adsorption energy and surface-P sp-band center as effective descriptors for the observed shift in selectivities across this series of TMPs. Furthermore, the calculated electronic-structure changes were found to exert greater influence over the observed product selectivity than the subtle geometric changes associated with lattice expansion. Identification of this structure–function relationship demonstrates that the controlled synthesis of TMPs enables an understanding of composition-dependent selectivity for the HDO reaction of phenolic molecules and this approach could be extended to other ternary TMP compositions for diverse catalytic applications. [ABSTRACT FROM AUTHOR]

Published
2023
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13. Compositional dependence of hydrodeoxygenation pathway selectivity for Ni2−xRhxP nanoparticle catalysts

Author

LiBretto, Nicole J., primary, Tacey, Sean A., additional, Zubair, Muhammad, additional, Bui, Tuong V., additional, Unocic, Kinga A., additional, Baddour, Frederick G., additional, Griffin, Michael B., additional, Schaidle, Joshua A., additional, Farberow, Carrie A., additional, Ruddy, Daniel A., additional, Bedford, Nicholas M., additional, and Habas, Susan E., additional

Published
2023
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22. Atomic Layer Deposition with TiO2 for Enhanced Reactivity and Stability of Aromatic Hydrogenation Catalysts

Author

McNeary, W. Wilson, primary, Tacey, Sean A., additional, Lahti, Gabriella D., additional, Conklin, Davis R., additional, Unocic, Kinga A., additional, Tan, Eric C. D., additional, Wegener, Evan C., additional, Erden, Tugce Eralp, additional, Moulton, Staci, additional, Gump, Chris, additional, Burger, Jessica, additional, Griffin, Michael B., additional, Farberow, Carrie A., additional, Watson, Michael J., additional, Tuxworth, Luke, additional, Van Allsburg, Kurt M., additional, Dameron, Arrelaine A., additional, Buechler, Karen, additional, and Vardon, Derek R., additional

Published
2021
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25. Optimizing Process Conditions during Catalytic Fast Pyrolysis of Pine with Pt/TiO2—Improving the Viability of a Multiple-Fixed-Bed Configuration

Author

French, Richard J., primary, Iisa, Kristiina, additional, Orton, Kellene A., additional, Griffin, Michael B., additional, Christensen, Earl, additional, Black, Stuart, additional, Brown, Kathleen, additional, Palmer, Scott E., additional, Schaidle, Joshua A., additional, Mukarakate, Calvin, additional, and Foust, Thomas D., additional

Published
2021
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26. Predicting thermal excursions during in situ oxidative regeneration of packed bed catalytic fast pyrolysis catalyst

Author

Adkins, Bruce D., primary, Mills, Zach, additional, Parks II, James, additional, Pecha, M. Brennan, additional, Ciesielski, Peter N., additional, Iisa, Kristiina, additional, Mukarakate, Calvin, additional, Robichaud, David J., additional, Smith, Kristin, additional, Gaston, Katherine, additional, Griffin, Michael B., additional, and Schaidle, Joshua A., additional

Published
2021
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28. Investigating deposition sequence during synthesis of Pd/Al2O3catalysts modified with organic monolayersElectronic supplementary information (ESI) available. See DOI: 10.1039/d1cy02131a

Author

Blanchette, Zachary, Zhang, Jing, Yazdi, Sadegh, Griffin, Michael B., Schwartz, Daniel K., and Medlin, J. Will

Abstract

Modification of supported metal catalysts with self-assembled monolayers (SAMs) has been shown to improve selectivity and turnover frequencies (TOFs) for many catalytic reactions. However, these benefits are often accompanied by a decrease in overall mass activity due to partial blocking of active sites by the monolayers. Therefore, a potential method for increasing site accessibility is to deposit the active metal (e.g., Pd) after deposition of a SAM modifier on the support material. In this work, Pd/Al2O3catalysts were synthesized using both a conventional, “metal-first” sequence in which the phosphonic acid (PA) SAM was deposited on Pd/Al2O3and a “SAM-first” technique in which the ligands were deposited onto the support prior to deposition of the metal. Although metal-first catalysts showed a significant increase in TOF during benzyl alcohol HDO, they exhibited only a modest increase in overall mass activity due to a decrease in the number of active sites. Meanwhile, SAM-first catalysts showed similar improvements in TOF and toluene selectivity but exhibited significantly improved HDO rates compared to metal-first catalysts. The rate increase was attributed to reduced site blocking as evidenced by CO chemisorption measurements. Additionally, analysis of catalysts having high Pd loadings using transmission electron microscopy (TEM) showed that SAM-first catalysts generally resulted in lower average particle sizes than traditionally modified and unmodified catalysts, suggesting that precoating the support surface with PAs changes the way that Pd is deposited during incipient wetness, leading here to improved activity.

Published
2022
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31. Driving towards cost-competitive biofuels through catalytic fast pyrolysis by rethinking catalyst selection and reactor configuration

Author

Griffin, Michael B., primary, Iisa, Kristiina, additional, Wang, Huamin, additional, Dutta, Abhijit, additional, Orton, Kellene A., additional, French, Richard J., additional, Santosa, Daniel M., additional, Wilson, Nolan, additional, Christensen, Earl, additional, Nash, Connor, additional, Van Allsburg, Kurt M., additional, Baddour, Frederick G., additional, Ruddy, Daniel A., additional, Tan, Eric C. D., additional, Cai, Hao, additional, Mukarakate, Calvin, additional, and Schaidle, Joshua A., additional

Published
2018
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