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<p>Conversion of polyethylene (PE) into high-value chemicals offers a sustainable approach to mitigate plastic pollution, yet achieving high selectivity and carbon efficiency remains a challenge. Herein, we report a one-pot method for converting PE into fatty di-carboxylic acids with a mass yield of 49%. Mechanistic insights derived from <i>in-situ</i> electron paramagnetic resonance (EPR), infrared (IR) spectroscopy, and small-molecule probe experiments reveal that PE oxidation proceeds through oxygen insertion driven by free radicals, followed by selective cleavage of carbon–carbon (C–C) bonds. A key distinction between catalytic and non-catalytic oxidation lies in the selective cleavage of carbonyl α-C bonds, which is dramatically enhanced by the manganese oxide (MnO<sub><i>x</i></sub>/SiO<sub>2</sub>) catalyst that drives the formation of fatty di-carboxylic acids while minimizing other by-products. In contrast, non-catalytic oxidation of PE follows a radical-mediated mechanism, yielding a broader product spectrum with lower selectivity for fatty di-carboxylic acids and reduced carbon efficiency. These findings underscore the need for integrated protocols balancing radical formation with catalyst-driven transformations, offering a foundation for advanced catalytic systems that improve both selectivity and efficiency in PE oxidation.</p>

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Mechanistic alteration of polyethylene oxidation via heterogenous catalysis for enhanced fatty di-carboxylic acid yields

  • 期刊论文

  • 发表日期：

    2025年7月10日

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  • Huidong Lv,
  • Yi Ji,
  • Wenjun Chen,
  • Yuan Xiang,
  • Yue Liu,
  • Jianrong Zeng,
  • Fei Huang,
  • Fan Zhang

摘要

Conversion of polyethylene (PE) into high-value chemicals offers a sustainable approach to mitigate plastic pollution, yet achieving high selectivity and carbon efficiency remains a challenge. Herein, we report a one-pot method for converting PE into fatty di-carboxylic acids with a mass yield of 49%. Mechanistic insights derived from in-situ electron paramagnetic resonance (EPR), infrared (IR) spectroscopy, and small-molecule probe experiments reveal that PE oxidation proceeds through oxygen insertion driven by free radicals, followed by selective cleavage of carbon–carbon (C–C) bonds. A key distinction between catalytic and non-catalytic oxidation lies in the selective cleavage of carbonyl α-C bonds, which is dramatically enhanced by the manganese oxide (MnOx/SiO2) catalyst that drives the formation of fatty di-carboxylic acids while minimizing other by-products. In contrast, non-catalytic oxidation of PE follows a radical-mediated mechanism, yielding a broader product spectrum with lower selectivity for fatty di-carboxylic acids and reduced carbon efficiency. These findings underscore the need for integrated protocols balancing radical formation with catalyst-driven transformations, offering a foundation for advanced catalytic systems that improve both selectivity and efficiency in PE oxidation.