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<p>Driven by the global plastic pollution crisis and the advancement of hydrogen energy strategies, efficient hydrogen production from waste plastics has emerged as a research hotspot. In this study, HDPE was employed as the feedstock, and a microwave-assisted catalytic pyrolysis technology integrated with a MIL-101(Fe)-derived Fe–C catalyst was developed for hydrogen production. The carbonization parameters of the catalyst were optimized, and multiple characterization techniques demonstrated that short-duration microwave treatment failed to induce the formation of the active magnetite (Fe<sub>3</sub>O<sub>4</sub>) phase. In contrast, prolonged treatment promoted the generation of more active sites, thereby improving catalytic performance. However, excessive carbonization led to a decrease in catalytic activity, which is attributed to the overcoating of Fe nanoparticles, densification of the carbon matrix, and overoxidation of active centers. Notably, a low-oxygen carbonization atmosphere favored the formation of Fe<sub>3</sub>O<sub>4</sub> and the generation of oxygen vacancies on the catalyst surface. Based on these findings, the optimal preparation conditions were determined as carbonization at 700&#xa0;°C for 1&#xa0;h under a low-oxygen atmosphere. Under these optimal conditions, the hydrogen (H<sub>2</sub>) yield and hydrogen conversion efficiency reached 49.2&#xa0;mmol/g<sub>HDPE</sub> and 77.2%, respectively. The reaction mechanism revealed that the catalyst absorbed microwave energy to initiate the cleavage of C–C bonds in HDPE within 2&#xa0;min, resulting in the formation of hydrocarbon intermediates and defective carbon deposits on the catalyst surface. The cleavage of C-H bonds occurred within 3–4&#xa0;min, leading to the rapid release of hydrogen.</p>

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Microwave-assisted catalytic hydrogen production from plastic pyrolysis over MOFs-derived Fe–C composite catalysts

  • 期刊论文

  • 发表日期：

    2026年2月4日

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  • Limin Hou,
  • Min Wang,
  • Jiaming Li,
  • Yihong Niu

摘要

Driven by the global plastic pollution crisis and the advancement of hydrogen energy strategies, efficient hydrogen production from waste plastics has emerged as a research hotspot. In this study, HDPE was employed as the feedstock, and a microwave-assisted catalytic pyrolysis technology integrated with a MIL-101(Fe)-derived Fe–C catalyst was developed for hydrogen production. The carbonization parameters of the catalyst were optimized, and multiple characterization techniques demonstrated that short-duration microwave treatment failed to induce the formation of the active magnetite (Fe3O4) phase. In contrast, prolonged treatment promoted the generation of more active sites, thereby improving catalytic performance. However, excessive carbonization led to a decrease in catalytic activity, which is attributed to the overcoating of Fe nanoparticles, densification of the carbon matrix, and overoxidation of active centers. Notably, a low-oxygen carbonization atmosphere favored the formation of Fe3O4 and the generation of oxygen vacancies on the catalyst surface. Based on these findings, the optimal preparation conditions were determined as carbonization at 700 °C for 1 h under a low-oxygen atmosphere. Under these optimal conditions, the hydrogen (H2) yield and hydrogen conversion efficiency reached 49.2 mmol/gHDPE and 77.2%, respectively. The reaction mechanism revealed that the catalyst absorbed microwave energy to initiate the cleavage of C–C bonds in HDPE within 2 min, resulting in the formation of hydrocarbon intermediates and defective carbon deposits on the catalyst surface. The cleavage of C-H bonds occurred within 3–4 min, leading to the rapid release of hydrogen.