Upcycling plastic waste into syngas by staged chemical looping gasification with modified Fe-based oxygen carriers

A novel staged approach, termed staged chemical looping gasification (SCLG) was proposed in this work, for the efficient upcycling of plastic waste into H2-rich syngas with exceptional carbon conversion reaching up to 99%. In such staged system, plastic was firstly pyrolyzed to generate hydrocarbon volatiles, followed by chemical looping reforming in the presence of oxygen carriers, and steam and air was also feed in sequence for carbon removal, syngas regulation and lattice oxygen recovery. A series of Fe-M-Al oxygen carriers (OCs, where M represents Mg, Ca, Mn, Mo, La, Ce) were synthesized and employed for SCLG of waste disposable masks. The performance and stability of these OCs were thoroughly investigated and compared in terms of H2 content and syngas production, while the physicochemical properties characterized by various techniques such as N2 isothermal adsorption-desorption, FESEM, XRD, TPO, and H2-TPR. Results showed that compared with the controlled Fe-Al sample, all the six modified OCs exhibited higher activity towards syngas production, due to the simultaneously enhanced both partial oxidation reactions and thermal decomposition reactions during the proposed SCLG process. However, the modifiers displayed different role for promoting gasification. Specifically, the addition of Ca significantly promoted the thermal cracking of plastic pyrolysis volatiles and lead to the deep extraction of carbon and H2, whereas the deposited carbon was further gasified into syngas in steam stage. As a result, Fe-Ca-Al showed the highest syngas yield and carbon conversion of 177.89 mmol/gOC and 99.03%, respectively. Fe-Mg-Al possessed relatively high CO selectivity, with the CO/(CO + CO2) ratio of 90.40%. The presence of MoO3 made the Fe-Mo-Al equipped with strong oxygen supply ability, leading to high content of oxygen-containing gases. Furthermore, the cycle stability of OCs was also conducted. The slight decrease in activity of Fe-Ca-Al was due to the metal sintering, whereas Fe-Mo-Al presented relatively stable syngas yield. The proposed staged chemical looping gasification with modified Fe-Al was demonstrated as a promising upcycling utilization of disposal plastic waste.