Pyrolysis of the Cellulose Fraction of Biomass in the Presence of Solid Acid Catalysts

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Pyrolysis of the Cellulose Fraction of Biomass in the Presence of Solid Acid Catalysts : An Operando Spectroscopy and Theoretical Investigation. / Keturakis, Christopher J.; Lapina, Olga B.; Shubin, Aleksandr A. et al.

In: ChemSusChem, Vol. 11, No. 23, 11.12.2018, p. 4044-4059.

Research output: Contribution to journal › Article › peer-review

BibTeX

@article{4f5a5844f3ea4b539c7740de43222405,

title = "Pyrolysis of the Cellulose Fraction of Biomass in the Presence of Solid Acid Catalysts: An Operando Spectroscopy and Theoretical Investigation",

abstract = "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 SiO2-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 AlOx nanostructures on SiO2 were determined with 27Al/1H 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 AlOx cluster and molecular nature of the biomass feedstock. These new insights allowed the establishment of fundamental structure–activity/selectivity relationships during biomass pyrolysis.",

keywords = "biomass, catalysts, operando spectroscopy, solid acid, supported AlO/SiO, MOLECULAR CHARACTERIZATION, LIGNOCELLULOSIC BIOMASS, supported Al2O3/SiO2, CARBONYL-COMPOUNDS, MECHANISMS, LEVOGLUCOSAN, GC-MS, PRODUCTS, PART 2, ELECTRIC-FIELD GRADIENTS, D-GLUCOSE",

author = "Keturakis, {Christopher J.} and Lapina, {Olga B.} and Shubin, {Aleksandr A.} and Terskikh, {Victor V.} and Evgeniy Papulovskiy and Yudaev, {Ivan V.} and Paukshtis, {Eugenii A.} and Wachs, {Israel E.}",

note = "{\textcopyright} 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.",

year = "2018",

month = dec,

day = "11",

doi = "10.1002/cssc.201802073",

language = "English",

volume = "11",

pages = "4044--4059",

journal = "ChemSusChem",

issn = "1864-5631",

publisher = "Wiley-VCH Verlag",

number = "23",

}

RIS

TY - JOUR

T1 - Pyrolysis of the Cellulose Fraction of Biomass in the Presence of Solid Acid Catalysts

T2 - An Operando Spectroscopy and Theoretical Investigation

AU - Keturakis, Christopher J.

AU - Lapina, Olga B.

AU - Shubin, Aleksandr A.

AU - Terskikh, Victor V.

AU - Papulovskiy, Evgeniy

AU - Yudaev, Ivan V.

AU - Paukshtis, Eugenii A.

AU - Wachs, Israel E.

PY - 2018/12/11

Y1 - 2018/12/11

N2 - 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 SiO2-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 AlOx nanostructures on SiO2 were determined with 27Al/1H 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 AlOx cluster and molecular nature of the biomass feedstock. These new insights allowed the establishment of fundamental structure–activity/selectivity relationships during biomass pyrolysis.

AB - 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 SiO2-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 AlOx nanostructures on SiO2 were determined with 27Al/1H 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 AlOx cluster and molecular nature of the biomass feedstock. These new insights allowed the establishment of fundamental structure–activity/selectivity relationships during biomass pyrolysis.

KW - biomass

KW - catalysts

KW - operando spectroscopy

KW - solid acid

KW - supported AlO/SiO

KW - MOLECULAR CHARACTERIZATION

KW - LIGNOCELLULOSIC BIOMASS

KW - supported Al2O3/SiO2

KW - CARBONYL-COMPOUNDS

KW - MECHANISMS

KW - LEVOGLUCOSAN

KW - GC-MS

KW - PRODUCTS

KW - PART 2

KW - ELECTRIC-FIELD GRADIENTS

KW - D-GLUCOSE

UR - http://www.scopus.com/inward/record.url?scp=85056797527&partnerID=8YFLogxK

U2 - 10.1002/cssc.201802073

DO - 10.1002/cssc.201802073

M3 - Article

C2 - 30338653

AN - SCOPUS:85056797527

VL - 11

SP - 4044

EP - 4059

JO - ChemSusChem

JF - ChemSusChem

SN - 1864-5631

IS - 23

ER -

ID: 17472204

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

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