Coupled conversion of polyethylene and carbon dioxide catalyzed by a zeolite-metal oxide system

沸石-金属氧化物体系催化聚乙烯与二氧化碳的耦合转化

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Abstract

Zeolite-catalyzed polyethylene (PE) aromatization achieves reduction of the aromatic yield via hydrogenation and hydrogenolysis reactions. The hydrogen required for CO(2) hydrogenation can be provided by H radicals formed during aromatization. In this study, we efficiently convert PE and CO(2) into aromatics and CO using a zeolite-metal oxide catalyst (HZSM-5 + CuZnZrO(x)) at 380°C and under hydrogen- and solvent-free reaction conditions. Hydrogen, derived from the aromatization of PE over HZSM-5, diffuses through the Brønsted acidic sites of the zeolite to the adjacent CuZnZrO(x), where it is captured in situ by CO(2) to produce bicarbonate and further hydrogenated to CO. This favors aromatization while inhibiting hydrogenation and secondary hydrogenolysis reactions. An aromatic yield of 62.5 wt % is achieved, of which 60% consisted of benzene, toluene, and xylene (BTX). The conversion of CO(2) reaches values as high as 0.55 mmol g(PE)(-1). This aromatization-hydrogen capture pathway provides a feasible scheme for the comprehensive utilization of waste plastics and CO(2).

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