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    废塑料与CO2协同催化转化制备高值产品研究进展

    Research Progress on Synergistic Catalytic Conversion of Waste Plastics and CO2 into High-Value Products

    • 摘要: 废塑料与CO2协同催化转化可同步实现固废资源化与温室气体消纳,是迈向碳循环经济的重要途径。本文综述了废塑料与CO2协同催化转化制备合成气、液体燃料(芳烃、低碳烯烃)、功能碳材料(多孔碳、碳纳米管)等技术路线。在高温(约800 ℃)条件下,可通过催化气化耦合废塑料裂解与CO2重整过程;CO2能够促进脱氢环化反应、抑制积炭生成,从而高效制备合成气。在约400 ℃中低温条件、金属氧化物/分子筛催化剂体系下,以CO2为氢清除剂,通过消耗塑料芳构化释放的氢物种促进芳烃生成,芳烃总产率可提升至75.3%。针对挥发分含量较高的聚烯烃塑料,可采用热解−催化−艺联产碳纳米管(CNTs)与高纯氢气;同时耦合CO2脱除无定形炭,进一步提高CNTs的纯度。此外,借助热解炭化耦合CO2活化造孔,可将含氧、含氯类塑料转化为多孔碳材料,所得产物在CO2捕集、水处理及储能领域具有广阔应用前景。本文总结了不同目标产物制备技术的特征与最新研究进展,探讨催化体系、反应工艺参数对产物选择性和产率的作用机制,并展望该领域未来发展。

       

      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.

       

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