Green Aromatics: Catalytic Valorisation of bio-derived 2,5-dimethylfuran over Zeolites and Zeotypes

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Sauer, Christopher,1993Chalmers tekniska högskola,Chalmers University of Technology (författare)

Green Aromatics: Catalytic Valorisation of bio-derived 2,5-dimethylfuran over Zeolites and Zeotypes

BokEngelska2022

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Gothenburg,2022
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LIBRIS-ID:oai:research.chalmers.se:361a9a33-a47e-4f7e-9150-6590b5a82b60
ISBN:9789179057466
https://research.chalmers.se/publication/533023URI

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Språk:engelska
Sammanfattning på:engelska

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This thesis discusses the use of biomass as a potentially green feedstock for the chemical industry in the urgent shift away from fossil resources. I elaborate on reasons why we cannot afford to burn virgin biomass for energy production, among them a variety of ecosystem services that forests and other lands provide. In addition, the utilisation of biomass should be focused on products that sequester and lock away carbon for more extended periods, e.g. timber, materials and chemicals. In particular, biomass can be used as an alternative "carbon neutral" feedstock for the chemical industry, where we can preserve the already existing chemical complexity in the bio-based molecules. One example is the upgrading of furans to benzene, toluene and xylene (BTX) aromatics with the help of zeolite catalysis. These aromatics are important commodity chemicals, where the shift to a bio-based resource could make use of already existing knowledge, catalyst and production infrastructure. However, research is necessary to understand these new feedstock molecules and their interaction with the catalysts and to enable the design of applicable catalysts. In order to study the interaction of the furans, in particular 2,5-dimethylfuran (2,5-dmf), I describe and discuss the development of an analytical methodology that utilises infrared spectroscopy and mass spectrometry for the on-line identification and quantification of product molecules during catalytic reactions. This on-line analysis method is then applied to the catalytic conversion of 2,5-dmf to aromatics over a range of zeolite and zeotype catalysts. In-depth studies with ammonia as a probe molecule of the catalytic active acid sites, as well as temperature programmed experiments with ammonia and 2,5-dmf give insights into product distribution, selectivity changes and deactivation of the catalyst. For example, olefins and aromatics are initially preferred products, while with increasing time on stream, the isomerisation of 2,5-dmf becomes dominant. The incorporation of Ga into the zeotype framework, resulting in a Ga-Silicate, shows how targeted catalyst design can increase overall aromatics production. This catalyst is also suitable for selective isomerisation of 2,5-dmf to 2,4-dimethylfuran, which has a rare substitution pattern. Finally, itwas found that the most valuable of BTX, p -xylene, can be produced more selectively when 2,5-dmf is pre-adsorbed onto zeolite ZSM-5 and then released during a temperature programmed product desorption.

Ämnesord och genrebeteckningar

NATURVETENSKAP Kemi Oorganisk kemi hsv//swe
NATURAL SCIENCES Chemical Sciences Inorganic Chemistry hsv//eng
NATURVETENSKAP Kemi Fysikalisk kemi hsv//swe
NATURAL SCIENCES Chemical Sciences Physical Chemistry hsv//eng
NATURVETENSKAP Kemi Analytisk kemi hsv//swe
NATURAL SCIENCES Chemical Sciences Analytical Chemistry hsv//eng
TEKNIK OCH TEKNOLOGIER Kemiteknik Kemiska processer hsv//swe
ENGINEERING AND TECHNOLOGY Chemical Engineering Chemical Process Engineering hsv//eng
NATURVETENSKAP Kemi Materialkemi hsv//swe
NATURAL SCIENCES Chemical Sciences Materials Chemistry hsv//eng
NATURVETENSKAP Kemi hsv//swe
NATURAL SCIENCES Chemical Sciences hsv//eng
NATURVETENSKAP Kemi Organisk kemi hsv//swe
NATURAL SCIENCES Chemical Sciences Organic Chemistry hsv//eng
Biomass conversion
infrared spectroscopy
BTX Aromatics
2,5-dimethylfuran
Zeolite
Catalysis
Online Analysis
Zeotype

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Chalmers tekniska högskola (creator_code:org_t)

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NATURVETENSKAP: NATURVETENSKAP; och Kemi; och Oorganisk kemi

NATURVETENSKAP: NATURVETENSKAP; och Kemi; och Fysikalisk kemi

NATURVETENSKAP: NATURVETENSKAP; och Kemi; och Analytisk kemi

TEKNIK OCH TEKNOLOGIER: TEKNIK OCH TEKNO ...; och Kemiteknik; och Kemiska processe ...

NATURVETENSKAP: NATURVETENSKAP; och Kemi; och Materialkemi

NATURVETENSKAP: NATURVETENSKAP; och Kemi

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NATURVETENSKAP: NATURVETENSKAP; och Kemi; och Organisk kemi

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