Hydrogen-free upcycling of polyethylene waste to methylated aromatics over Ni/ZSM-5 under mild conditions

Upcycling waste plastic into aromatics presents an attractive strategy to tackle both plastic pollution and energy challenges. However, previous studies often rely on high temperatures, precious metals, and have broad product distributions. In this study, we reported that a Ni/ZSM-5 bifunctional catalyst can directly convert polyethylene (PE) into methylated aromatics with high selectivity under mild conditions, while eliminating the requirement for hydrogen gas and solvents. The liquid yield could attain up to 70.3%, and the aromatics yield could achieve up to 51.7%. Over 78.4% of the aromatics were methylated aromatics including toluene, xylene, and mesitylene. Polymer chains underwent dehydrogenation over Ni and the acid sites in ZSM-5, forming C=C bonds. Certain of these bonds evolved into carbenium ions through the process of proton transfer at the acid sites. The optimization of Ni and acid sites enhanced the oligomerization, cyclization, and aromatization process. The extra mesopores created by Ni on the molecular sieve aid in the generation of aromatics. Furthermore, the Ni/ZSM-5 catalyst demonstrated the ability to convert typical commercial grades of PE plastic, such as gloves and bottles, into aromatics with a selectivity of up to 61.1%. It offers an economically feasible and environmentally friendly upcycling avenue for the circular economy of plastics.