The present invention relates to a novel process for the preparation of low molecular weight aromatic compounds such as benzene, toluene, and xylenes (BTX) from plastics. Provided is a thermo-catalytic pyrolysis process for the preparation of aromatic compounds from a feed stream comprising plastic, comprising the steps of: a) subjecting a feed stream comprising a plastic to a pyrolysis treatment at a pyrolysis temperature in the range of 600-1000°C to produce pyrolysis vapors; b) optionally cooling the pyrolysis vapors to a temperature that is below the pyrolysis temperature; c) contacting the vaporous phase with an aromatization catalyst at an aromatization temperature in the range of 450 - 700 °C, which aromatization temperature is at least 50°C lower than the pyrolysis temperature, in a catalytic conversion step to yield a conversion product comprising aromatic compounds; and d) optionally recovering the aromatic compounds from the conversion product.
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The catalytic coconversion of glycerol and toluene (93/7 wt %) over a technical H-ZSM-5/Al2O3 (60-40 wt %) catalyst was studied, aiming for enhanced production of biobased benzene, toluene, and xylenes (bio-BTX). When using glycerol/toluene cofeed with a mass ratio of 93/7 wt %, a peak BTX carbon yield of 29.7 ± 1.1 C.% (at time on stream (TOS) of 1.5-2.5 h), and an overall BTX carbon yield of 28.7 C.% (during TOS of 8.5 h) were obtained, which are considerably higher than those (19.1 ± 0.4 C.% and 11.0 C.%) for glycerol alone. Synergetic effects when cofeeding toluene on the peak and overall BTX carbon yields were observed and quantified, showing a relative increase of 3.1% and 30.0% for the peak and overall BTX carbon yield (based on the feedstock). These findings indicate that the strategy of cofeeding in situ produced toluene for the conversion of glycerol to aromatics has potential to increase BTX yields. In addition, BTX production on the catalyst (based on the fresh catalyst during the first run for TOS of 8.5 h and without regeneration) is significantly improved to 0.547 ton ton-1catalyst (excluding the 76% of toluene product that is 0.595 ton ton-1catalyst for the recycle in the cofeed) for glycerol/toluene cofeed, which was 0.426 ton ton-1catalyst for glycerol alone. In particular, this self-sufficient toluene product recycling strategy is advantageous for the production and selectivity (relative increase of 84.4% and 43.5% during TOS of 8.5 h) of biobased xylenes.
Sustainable production of aromatics, especially benzene, toluene and xylenes (BTX), is essential considering their broad applications and the current global transition away from crude oil utilization. Aromatization of lower olefins, particularly ethene and propene, offers great potential if they are derived from more circular alternative carbon feedstocks such as biomass and waste plastics. This work aims to identify the preferred olefin feed, ethene or propene, for BTX production in a fixed-bed reactor. A commercial H-ZSM-5 (Si/Al = 23) catalyst was used as a reference catalyst, as well as a Ga-ZSM-5 catalyst, prepared by Ga ion-exchange of the H-ZSM-5 catalyst. At 773 K, 1 bar, 45 vol % olefin, 6.75 h−1, propene aromatization over the Ga-ZSM-5 catalyst exhibited higher BTX selectivity of 55 % and resulted in slower catalyst deactivation compared to ethene aromatization.
Paper sludge contains papermaking mineral additives and fibers, which could be reused or recycled, thus enhancing the circularity. One of the promising technologies is the fast pyrolysis of paper sludge, which is capable of recovering > 99 wt.% of the fine minerals in the paper sludge and also affording a bio-liquid. The fine minerals (e.g., ‘circular’ CaCO3) can be reused as filler in consumer products thereby reducing the required primary resources. However, the bio-liquid has a lower quality compared to fossil fuels, and only a limited application, e.g., for heat generation, has been applied. This could be significantly improved by catalytic upgrading of the fast pyrolysis vapor, known as an ex-situ catalytic pyrolysis approach. We have recently found that a high-quality bio-oil (mainly ‘bio-based’ paraffins and low-molecular-weight aromatics, carbon yield of 21%, and HHV of 41.1 MJ kg-1) was produced (Chem. Eng. J., 420 (2021), 129714). Nevertheless, catalyst deactivation occurred after a few hours’ of reaction. As such, catalyst stability and regenerability are of research interest and also of high relevance for industrial implementation. This project aims to study the potential of the add-on catalytic upgrading step to the industrial fast pyrolysis of paper sludge process. One important performance metric for sustainable catalysis in the industry is the level of catalyst consumption (kgcat tprod-1) for catalytic pyrolysis of paper sludge. Another important research topic is to establish the correlation between yield and selectivity of the bio-chemicals and the catalyst characteristics. For this, different types of catalysts (e.g., FCC-type E-Cat) will be tested and several reaction-regeneration cycles will be performed. These studies will determine under which conditions catalytic fast pyrolysis of paper sludge is technically and economically viable.
