Correction: Unravelling potential reaction intermediates during catalytic pyrolysis of polypropylene with microscopy and spectroscopy.

[This corrects the article DOI: 10.1039/D3CY01473H.].

Unravelling potential reaction intermediates during catalytic pyrolysis of polypropylene with microscopy and spectroscopy.

While plastics-to-plastics recycling via melting and re-extrusion is often the preferred option due to a relatively low CO2 footprint, this technique requires a highly sorted waste stream and plastic properties can often not be maintained. Obtaining aromatics, such as benzene, toluene, and xylene (BTX), via catalytic pyrolysis of polyolefins, such as polypropylene and polyethylene, offers another attractive recycling technology. In this process, a discarded crude oil refinery catalyst (ECAT) was previously shown to lower the unwanted formation of deactivating coke species compared to a fresh crude oil refinery catalyst (FCC-cat), while yielding 20 wt% aromatics from polypropylene. In this work, we study the underlying reaction mechanism for this chemical recycling process over the fresh and used refinery catalyst as well as a model system, not containing any zeolite material, using a combination of microscopy and spectroscopy. More specifically, by using in situ fluorescence microscopy, in situ infrared spectroscopy, in situ ultraviolet-visible spectroscopy as well as ex situ solid-state nuclear magnetic resonance, we observe highly fluorescent methylated aromatic intermediates that differ for the three catalyst materials under study both in their fluorescence, IR, UV-vis, and NMR spectroscopy features. This detailed micro-spectroscopic comparison informs which potential reaction intermediates lead to increased coke formation. Our results suggests that a next generation of catalyst materials for this process would profit from a higher accessibility and a milder acidity compared to an FCC-cat and shows the great potential of using ECAT to reduce coking and obtain a BTX stream, which could be become the chemical building blocks for the manufacturing of e.g., plastics and coating materials.

Plastic Waste Conversion over a Refinery Waste Catalyst.

Polypropylene (PP) makes up a large share of our plastic waste. We investigated the conversion of PP over the industrial Fluid Catalytic Cracking catalyst (FCC-cat) used to produce gasoline from crude oil fractions. We studied transport limitations arising from the larger size of polymers compared to the crude oil-based feedstock by testing the components of this catalyst separately. Infrared spectroscopy and confocal fluorescence microscopy revealed the role of the FCC matrix in aromatization, and the zeolite Y domains in coking. An equilibrium catalyst (ECAT), discarded during FCC operation as waste, produced the same aromatics content as a fresh FCC-cat, while coking decreased significantly, likely due to the reduced accessibility and activity of the zeolite domains and an enhanced cracking activity of the matrix due to metal deposits present in ECAT. This mechanistic understanding provides handles for further improving the catalyst composition towards higher aromatics selectivity.

Beyond Mechanical Recycling: Giving New Life to Plastic Waste.

Increasing the stream of recycled plastic necessitates an approach beyond the traditional recycling via melting and re-extrusion. Various chemical recycling processes have great potential to enhance recycling rates. In this Review, a summary of the various chemical recycling routes and assessment via life-cycle analysis is complemented by an extensive list of processes developed by companies active in chemical recycling. We show that each of the currently available processes is applicable for specific plastic waste streams. Thus, only a combination of different technologies can address the plastic waste problem. Research should focus on more realistic, more contaminated and mixed waste streams, while collection and sorting infrastructure will need to be improved, that is, by stricter regulation. This Review aims to inspire both science and innovation for the production of higher value and quality products from plastic recycling suitable for reuse or valorization to create the necessary economic and environmental push for a circular economy.