Pyrolysis of the Cellulose Fraction of Biomass in the Presence of Solid Acid Catalysts: An Operando Spectroscopy and Theoretical Investigation.

Autor: Keturakis CJ; Operando Molecular Spectroscopy & Catalysis Research Laboratory, Department of Chemical Engineering, Lehigh University, Bethlehem, PA, 18015, USA.; Current address: Cummins Emission Solutions, Stoughton, WI, 53589, USA., Lapina OB; Boreskov Institute of Catalysis, pr. Lavrentieva, 5, 630090, Novosibirsk, Russia.; Novosibirsk State University, Pirogova, 2, 630090, Novosibirsk, Russia., Shubin AA; Boreskov Institute of Catalysis, pr. Lavrentieva, 5, 630090, Novosibirsk, Russia.; Novosibirsk State University, Pirogova, 2, 630090, Novosibirsk, Russia., Terskikh VV; Department of Chemistry, University of Ottawa, Ottawa, Ontario, K1N6N5, Canada., Papulovskiy E; Boreskov Institute of Catalysis, pr. Lavrentieva, 5, 630090, Novosibirsk, Russia., Yudaev IV; Boreskov Institute of Catalysis, pr. Lavrentieva, 5, 630090, Novosibirsk, Russia., Paukshtis EA; Boreskov Institute of Catalysis, pr. Lavrentieva, 5, 630090, Novosibirsk, Russia.; Novosibirsk State University, Pirogova, 2, 630090, Novosibirsk, Russia., Wachs IE; Operando Molecular Spectroscopy & Catalysis Research Laboratory, Department of Chemical Engineering, Lehigh University, Bethlehem, PA, 18015, USA.
Jazyk: angličtina
Zdroj: ChemSusChem [ChemSusChem] 2018 Dec 11; Vol. 11 (23), pp. 4044-4059. Date of Electronic Publication: 2018 Nov 19.
DOI: 10.1002/cssc.201802073
Abstrakt: Biomass pyrolysis by solid acid catalysts is one of many promising technologies for sustainable production of hydrocarbon liquid fuels and value-added chemicals, but these complex chemical transformations are still poorly understood. A series of well-defined model SiO 2 -supported alumina catalysts were synthesized and molecularly characterized, under dehydrated conditions and during biomass pyrolysis, with the aim of establishing fundamental catalyst structure-activity/selectivity relationships. The nature and corresponding acidity of the supported AlO x nanostructures on SiO 2 were determined with 27 Al/ 1 H NMR and IR spectroscopy of chemisorbed CO, and DFT calculations. Operando time-resolved IR-Raman-MS spectroscopy studies revealed the molecular transformations taking place during biomass pyrolysis. The molecular transformations during biomass pyrolysis depended on both the domain size of the AlO x cluster and molecular nature of the biomass feedstock. These new insights allowed the establishment of fundamental structure-activity/selectivity relationships during biomass pyrolysis.
(© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)
Databáze: MEDLINE