Tailoring ZSM‐5 Zeolites for the Fast Pyrolysis of Biomass to Aromatic Hydrocarbons

Hoff, Thomas C.; Gardner, David P.; Thilakaratne, Rajeeva; Wang, Kaige; Hansen, Thomas Willum; Brown, Robert C.; Tessonnier, Jean Philippe

doi:10.1002/cssc.201600186

Cited by 64 publications

(46 citation statements)

References 50 publications

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“…It is important to note here, especially considering the following catalysis part, that the presence of mesopores is not the sole important parameter to respect. Indeed, a certain preservation of the initial microporous network is essential too [43]. In other terms, the connectivity between the transport-responsible mesopores and catalysis-responsible micropores is important and will be evaluated later by the catalytic results.…”

Section: Characterisationmentioning

confidence: 99%

Mesoporous ZSM-5 Zeolites in Acid Catalysis: Top-Down vs. Bottom-Up Approach

et al. 2017

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Abstract:A top-down desilication of Al-rich ZSM-5 zeolites and a bottom-up mesopores creating method were evaluated in this study. Three liquid-solid and one gas-solid heterogeneously-catalysed reactions were chosen to establish relationships between zeolites textural properties and their catalytic behavior in acid-catalysed model reactions that are influenced by shape selectivity: Diels-Alder cyclization between isoprene and methylacrylate, Methanol-to-Olefins (MTO) reaction, chlorination of iodobenzene with trichloroisocyanuric acid (TCCA), and Friedel-Crafts acylation of anisole by carboxylic acids with differing sizes. It is found amongst others that no optimal mesoporosity for all the different reactions can be easily obtained, but depending on the chosen application, a specific treatment has to be set to achieve high activity/selectivity and stability.

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Section: Characterisationmentioning

confidence: 99%

Mesoporous ZSM-5 Zeolites in Acid Catalysis: Top-Down vs. Bottom-Up Approach

et al. 2017

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“…However, oxides depolymerization capacity is known to be lower when compared to other catalysts, such as zeolites . By opposition, zeolite suffers fast deactivation due to the condensation of the highly reactive FP oxygenated intermediates inside the zeolite crystalline structure leading to coke formation. Therefore, the deposition of spinel oxide particles, such as MgFe 2 O 4 , in the external surface of the zeolite crystal would enable preliminary deoxygenation of the pyrolysis vapours, thus improving the overall zeolite potential.…”

Section: Resultsmentioning

confidence: 99%

“…ZSM‐5 stands out as the most favourable choice of zeolite due to its inherently well‐defined MFI pore structure for shape selective production of aromatic hydrocarbons . Nonetheless, the fast pyrolysis intermediate products suffer diffusion limitations on ZSM‐5 crystalline porous framework thereby undergoing over‐cracking and producing coke that results into catalyst deactivation by pore blockage and reduction of available catalytic actives due to coverage (active site poisoning) . Moreover, a large amount of water vapour in bio oils also leads to dealumination of the zeolite materials, which in turn leads to loss of surface area and irreversible deactivation of the zeolite .…”

Section: Introductionmentioning

confidence: 99%

Hybridization of ZSM‐5 with Spinel Oxides for Biomass Vapour Upgrading

et al. 2020

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In this study, we report catalytic fast pyrolysis of biomass using multifunctional hybrid spinel‐oxide@zeolite catalysts prepared by using the steam‐assisted crystallization (SAC) method to create the mesoporous zeolite followed by urea hydrolysis of metal nitrates to deposit spinel‐oxides. This hybrid catalyst was quite effective in the deoxygenation of pinewood sawdust pyrolysis vapours, while avoiding over cracking of the lignin precursors, which are already ideal as chemical and fuel precursors. In the first step, multiple spinel oxides MgB2O4 (where B=Fe, Al, Ce, Ga, Cr) were screened as catalysts for the pyrolysis of pinewood sawdust and the resultant bio‐oil (bio‐oil on the water‐free basis) was assessed in terms of carbon efficiency, oxygen content and chemical composition. While all the tested spinel oxides deoxygenated the pyrolysis vapour, MgAl2O4 and MgFe2O4 were found to provide a well‐balanced deoxygenation degree and producing bio‐oil with acceptable carbon efficiency. Catalytic activity and product distribution were affected by the density and strength of the acid sites of the spinel oxides. Subsequently, CFP over MgFe2O4@ZSM5 and MgAl2O4@ZSM5 was investigated under similar condition. The better performance of the hybrid catalyst was attributed to the deposition of small particles of MgFe2O4 in the external surface of the zeolite. The presence of this spinel oxide on the external surface depolymerized bulky oxygenates to lighter fractions that could easily access the active sites within the mesoporous structure of the zeolite, thus providing the catalytic function needed for the oxygen removal after aromatic ring saturation.

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“…When the temperature was high enough (> 250 o C), the biomass sample started to decompose into the pyrolysis vapor and char, and then the pyrolysis vapor passed through catalysts. In the instant contact between the pyrolysis vapor and the catalyst, the pyrolysis intermediates were converted into aromatic hydrocarbons [45]. The diffusional resistances became predominant for the catalysts' micropores, which could lower the releasing speed of the pyrolysis volatile products in comparison to non-catalytic pyrolysis.…”

Section: Resultsmentioning

confidence: 99%

Reaction chemistry and kinetics of corn stalk pyrolysis without and with Ga/HZSM-5

Huang

Xie

Yang

et al. 2018

J Therm Anal Calorim

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The bifunctional Ga/HZSM-5 catalyst has been proven having the capabiliity to increase the selectivity of aromatics production during catalytic pyrolysis of furan and woody biomass. However, the reaction chemistry and kinetics of pyrolysis of herbaceous biomass promoted by Ga/HZSM-5 is rarely reported. Pyrolysisgas chromatography / mass spectrometry (Py-GC/MS) analysis and nonisothermal thermogravimetric (TG) analysis at four heating rates were carried out to investigate the decomposition behavior and pyrolysis kinetics of corn stalk without and with Ga/HZSM-5. The effective activation energies for corn stalk pyrolysis were calculated by using the Friedman isoconversional method. The Py-GC/MS analysis results indicated that the Ga/HZSM-5 catalyst had a high selectivity towards producing the aromatic chemicals of xylene, toluene and benzene, whereas the major products from noncatalytic pyrolysis of corn stalk were oxygenated compounds. The presence of Ga/HZSM-5 could significantly reduce the effective activation energies of corn stalk pyrolysis from 159.9-352.4 kJ mol-1 to 41.6-99.8 kJ mol-1 in the conversion range of 0.10-0.85.

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Tailoring ZSM‐5 Zeolites for the Fast Pyrolysis of Biomass to Aromatic Hydrocarbons

Cited by 64 publications

References 50 publications

Mesoporous ZSM-5 Zeolites in Acid Catalysis: Top-Down vs. Bottom-Up Approach

Mesoporous ZSM-5 Zeolites in Acid Catalysis: Top-Down vs. Bottom-Up Approach

Hybridization of ZSM‐5 with Spinel Oxides for Biomass Vapour Upgrading

Reaction chemistry and kinetics of corn stalk pyrolysis without and with Ga/HZSM-5

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