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Catalytic fast pyrolysis of biomass : catalyst characterization reveals the feed-dependent deactivation of a technical ZSM-5-based catalyst

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Abstract
Catalyst deactivation due to coking is a major challenge in the catalytic fast pyrolysis (CFP) of biomass. Here, a multitechnique investigation of a technical Al2O3-bound ZSM-5-based extrudate catalyst, used for the CFP of pine wood and cellulose (at a reactor temperature of 500 °C), provided insight into the effects of extrusion, the catalytic pyrolysis process, and catalyst regeneration on the catalyst structure. As a result of a reduction in acidity and surface area due to the coking catalyst, the activity dropped drastically with increasing time-on-stream (TOS), as evidenced by a decrease in aromatics yield. Strikingly, confocal fluorescence microscopy at the single-particle level revealed that vapor components derived from whole biomass or just the cellulose component coke differently. While pine-wood-derived species mainly blocked the external area of the catalyst particle, larger carbon deposits were formed inside the catalyst’s micropores with cellulose-derived species. Pyridine FT-IR and solid-state NMR spectroscopy demonstrated irreversible changes after regeneration, likely due to partial dealumination. Taken together with <30 g kg–1 aromatics yield on a feed basis, the results show a mismatch between biomass pyrolysis vapors and the technical catalyst used due to a complex interplay of mass transfer limitations and CFP chemistry.
Keywords
Catalytic pyrolysis, Biomass, Zeolite ZSM-5, Alumina, BTX, Spectroscopy, Catalyst deactivation, NUCLEAR-MAGNETIC-RESONANCE, METHANOL-TO-HYDROCARBONS, BIO-OIL, UV/VIS MICROSPECTROSCOPY, HZSM-5 ZEOLITE, COKE FORMATION, ZSM-5, CRACKING, PINE, TEMPERATURE

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MLA
Luna-Murillo, Beatriz, et al. “Catalytic Fast Pyrolysis of Biomass : Catalyst Characterization Reveals the Feed-Dependent Deactivation of a Technical ZSM-5-Based Catalyst.” ACS SUSTAINABLE CHEMISTRY & ENGINEERING, vol. 9, no. 1, 2021, pp. 291–304, doi:10.1021/acssuschemeng.0c07153.
APA
Luna-Murillo, B., Pala, M., Paioni, A. L., Baldus, M., Ronsse, F., Prins, W., … Weckhuysen, B. M. (2021). Catalytic fast pyrolysis of biomass : catalyst characterization reveals the feed-dependent deactivation of a technical ZSM-5-based catalyst. ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 9(1), 291–304. https://doi.org/10.1021/acssuschemeng.0c07153
Chicago author-date
Luna-Murillo, Beatriz, Mehmet Pala, Alessandra Lucini Paioni, Marc Baldus, Frederik Ronsse, Wolter Prins, Pieter C. A. Bruijnincx, and Bert M. Weckhuysen. 2021. “Catalytic Fast Pyrolysis of Biomass : Catalyst Characterization Reveals the Feed-Dependent Deactivation of a Technical ZSM-5-Based Catalyst.” ACS SUSTAINABLE CHEMISTRY & ENGINEERING 9 (1): 291–304. https://doi.org/10.1021/acssuschemeng.0c07153.
Chicago author-date (all authors)
Luna-Murillo, Beatriz, Mehmet Pala, Alessandra Lucini Paioni, Marc Baldus, Frederik Ronsse, Wolter Prins, Pieter C. A. Bruijnincx, and Bert M. Weckhuysen. 2021. “Catalytic Fast Pyrolysis of Biomass : Catalyst Characterization Reveals the Feed-Dependent Deactivation of a Technical ZSM-5-Based Catalyst.” ACS SUSTAINABLE CHEMISTRY & ENGINEERING 9 (1): 291–304. doi:10.1021/acssuschemeng.0c07153.
Vancouver
1.
Luna-Murillo B, Pala M, Paioni AL, Baldus M, Ronsse F, Prins W, et al. Catalytic fast pyrolysis of biomass : catalyst characterization reveals the feed-dependent deactivation of a technical ZSM-5-based catalyst. ACS SUSTAINABLE CHEMISTRY & ENGINEERING. 2021;9(1):291–304.
IEEE
[1]
B. Luna-Murillo et al., “Catalytic fast pyrolysis of biomass : catalyst characterization reveals the feed-dependent deactivation of a technical ZSM-5-based catalyst,” ACS SUSTAINABLE CHEMISTRY & ENGINEERING, vol. 9, no. 1, pp. 291–304, 2021.
@article{8686187,
  abstract     = {{Catalyst deactivation due to coking is a major challenge in the catalytic fast pyrolysis (CFP) of biomass. Here, a multitechnique investigation of a technical Al2O3-bound ZSM-5-based extrudate catalyst, used for the CFP of pine wood and cellulose (at a reactor temperature of 500 °C), provided insight into the effects of extrusion, the catalytic pyrolysis process, and catalyst regeneration on the catalyst structure. As a result of a reduction in acidity and surface area due to the coking catalyst, the activity dropped drastically with increasing time-on-stream (TOS), as evidenced by a decrease in aromatics yield. Strikingly, confocal fluorescence microscopy at the single-particle level revealed that vapor components derived from whole biomass or just the cellulose component coke differently. While pine-wood-derived species mainly blocked the external area of the catalyst particle, larger carbon deposits were formed inside the catalyst’s micropores with cellulose-derived species. Pyridine FT-IR and solid-state NMR spectroscopy demonstrated irreversible changes after regeneration, likely due to partial dealumination. Taken together with <30 g kg–1 aromatics yield on a feed basis, the results show a mismatch between biomass pyrolysis vapors and the technical catalyst used due to a complex interplay of mass transfer limitations and CFP chemistry.}},
  author       = {{Luna-Murillo, Beatriz and Pala, Mehmet and Paioni, Alessandra Lucini and Baldus, Marc and Ronsse, Frederik and Prins, Wolter and Bruijnincx, Pieter C. A. and Weckhuysen, Bert M.}},
  issn         = {{2168-0485}},
  journal      = {{ACS SUSTAINABLE CHEMISTRY & ENGINEERING}},
  keywords     = {{Catalytic pyrolysis,Biomass,Zeolite ZSM-5,Alumina,BTX,Spectroscopy,Catalyst deactivation,NUCLEAR-MAGNETIC-RESONANCE,METHANOL-TO-HYDROCARBONS,BIO-OIL,UV/VIS MICROSPECTROSCOPY,HZSM-5 ZEOLITE,COKE FORMATION,ZSM-5,CRACKING,PINE,TEMPERATURE}},
  language     = {{eng}},
  number       = {{1}},
  pages        = {{291--304}},
  title        = {{Catalytic fast pyrolysis of biomass : catalyst characterization reveals the feed-dependent deactivation of a technical ZSM-5-based catalyst}},
  url          = {{http://dx.doi.org/10.1021/acssuschemeng.0c07153}},
  volume       = {{9}},
  year         = {{2021}},
}

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