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<p>A gap in understanding the deactivation mechanisms underlying heterogeneous catalytic advanced oxidation processes (HG-AOPs) constrains their sustainable development. This study clarifies the linkage between polymerization phenomena and catalyst deactivation in HG-AOPs employing carbon materials. We demonstrate that the deposition of polymerization products leads to a self-inhibition effect by maintaining a consistent polymerization energy barrier, regardless of the increasing degree of polymerization (DP). This consistency facilitates the persistent formation of high-DP products. Using machine learning analysis, we reveal that higher DPs intensify hydrophobic interactions and van der Waals forces, which promote the robust adhesion of polymeric products to the catalyst surface. These adherent layers compete with oxidants for active sites, impeding oxidant adsorption, obstructing electron transfer and ultimately hindering further catalytic activity. Additionally, we evaluate several catalyst-regeneration methods from a sustainability standpoint. This work contributes to developing sustainable strategies for effectively utilizing carbon-based nanomaterials in water treatment, offering a foundation for future innovation in HG-AOPs.</p>

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Polymeric products deactivate carbon-based catalysts in catalytic oxidation reactions

  • 期刊论文

  • 发表日期：

    2025年1月17日

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  • Pi-Jun Duan,
  • Jiu-Yun Liu,
  • Lei Chen,
  • Ming-Xue Li,
  • Jing-Wen Pan,
  • Zhi-Quan Zhang,
  • Chang-Wei Bai,
  • Xin-Jia Chen,
  • Han-Qing Yu,
  • Fei Chen

摘要

A gap in understanding the deactivation mechanisms underlying heterogeneous catalytic advanced oxidation processes (HG-AOPs) constrains their sustainable development. This study clarifies the linkage between polymerization phenomena and catalyst deactivation in HG-AOPs employing carbon materials. We demonstrate that the deposition of polymerization products leads to a self-inhibition effect by maintaining a consistent polymerization energy barrier, regardless of the increasing degree of polymerization (DP). This consistency facilitates the persistent formation of high-DP products. Using machine learning analysis, we reveal that higher DPs intensify hydrophobic interactions and van der Waals forces, which promote the robust adhesion of polymeric products to the catalyst surface. These adherent layers compete with oxidants for active sites, impeding oxidant adsorption, obstructing electron transfer and ultimately hindering further catalytic activity. Additionally, we evaluate several catalyst-regeneration methods from a sustainability standpoint. This work contributes to developing sustainable strategies for effectively utilizing carbon-based nanomaterials in water treatment, offering a foundation for future innovation in HG-AOPs.