Abstract:
Background The synergistic catalytic conversion of waste plastics and CO2 simultaneously enables the resource utilization of solid waste and the fixation of greenhouse gases, representing an important pathway toward a carbon circular economy.
Objective This paper aims to systematically review technical routes for the coupled catalytic conversion of waste plastics and CO2 into syngas, liquid fuels, high-value chemicals (aromatics and light olefins), and functional carbon materials (porous carbon and carbon nanotubes).
Progress At high temperatures (~800 °C), the cracking of waste plastics is coupled with CO2 reforming via catalytic gasification, in which CO2 promotes dehydrocyclization while suppressing carbon deposition, enabling the efficient production of syngas. CO2 can dissociate on the catalyst surface to generate reactive oxygen species, which facilitate the activation and reforming of C–H/C–C bonds in plastic-derived volatiles. At low-to-medium temperatures (~400 °C), over metal oxide/zeolite catalysts, CO2 serves as a hydrogen scavenger, consuming the hydrogen species released during plastic aromatization and thereby promoting aromatic formation, with the total aromatic yield reaching up to 75.3 wt%. Building on a single-zeolite system, the introduction of metal oxides can effectively capture these hydrogen species released during aromatization, thereby coupling aromatization with CO2 conversion. The co-conversion of waste plastics and CO2 not only enables the production of syngas and chemicals, but also facilitates the transformation of waste plastics into functional carbon materials. For polyolefin plastics with high volatile matter content, a tandem pyrolysis-catalytic process enables the co-production of carbon nanotubes (CNTs) and high-purity hydrogen. The plastic volatiles undergo cracking and carbon rearrangement over transition metal catalysts such as Ni, Fe, and Co, leading to the in situ growth of CNTs, while the introduction of CO2 further removes amorphous carbon to improve CNT purity. In addition, by coupling pyrolytic carbonization with CO2 activation for pore generation, oxygen- and chlorine-containing plastics can be converted into porous carbon with a high specific surface area and abundant pore structures, offering broad application prospects in CO2 capture, water treatment, and energy storage. CO2 can be directly introduced into the carbon preparation process to react with carbon atoms and etch the carbon framework, enabling the formation of pores both on the surface and within the carbon material.
Conclusions This work summarizes the characteristics of target products and recent advances in their preparation techniques, and discusses the mechanistic roles of catalytic systems and reaction process parameters in governing product selectivity and yield, providing theoretical and technical references for the development of novel low-carbon solid waste disposal and greenhouse gas resource utilization technologies.