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<p>Accumulation of plastic waste presents a global environmental crisis, posing severe threats to ecosystems. Depolymerization offers a promising route for closed-loop recycling of plastic waste. Nevertheless, depolymerizing chemically stable polyolefins remains challenging, yet fails to achieve high light olefin yields and stability. Herein, we propose an interfacial configurational entropy tuning strategy for liquid alloy catalysts, inducing active site interfacial enrichment and optimizing electronic structure. With this strategy, a quaternary GaInNiSn catalyst with medium entropy is developed for recycling polyolefins into light olefins under atmospheric pressure without co-reactant consumption, achieving a space-time yield of 181.5 mmol g<sub>cat</sub>⁻<sup>1</sup> h⁻<sup>1</sup>. Mechanistic insights reveal that Ni<sup><i>δ</i></sup>⁻–Sn<sup><i>δ</i>+</sup> active sites form within the dynamic Ga interface, enabling C–H bond activation to promote β-scission. Furthermore, a photovoltaics-driven depolymerization system is constructed, maintaining light olefin output of 52.8 L h⁻<sup>1</sup> over 120 hours. Our work unlocks a potent tool for efficient and sustainable plastic waste utilization.</p>

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Interfacial configurational entropy tuning strategy enabling liquid alloys for efficient depolymerization of polyolefin waste

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年3月12日

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  • Chaoping Xu,
  • Haoyu Yan,
  • Pengxuan Wang,
  • Jun Li,
  • Haihao Wen,
  • Xiaonan Wang,
  • Jiaming Ma,
  • Qian Zhang,
  • Xiao Zhang,
  • Dawei Tang,
  • Bo Jiang

摘要

Accumulation of plastic waste presents a global environmental crisis, posing severe threats to ecosystems. Depolymerization offers a promising route for closed-loop recycling of plastic waste. Nevertheless, depolymerizing chemically stable polyolefins remains challenging, yet fails to achieve high light olefin yields and stability. Herein, we propose an interfacial configurational entropy tuning strategy for liquid alloy catalysts, inducing active site interfacial enrichment and optimizing electronic structure. With this strategy, a quaternary GaInNiSn catalyst with medium entropy is developed for recycling polyolefins into light olefins under atmospheric pressure without co-reactant consumption, achieving a space-time yield of 181.5 mmol gcat⁻1 h⁻1. Mechanistic insights reveal that Niδ⁻–Snδ+ active sites form within the dynamic Ga interface, enabling C–H bond activation to promote β-scission. Furthermore, a photovoltaics-driven depolymerization system is constructed, maintaining light olefin output of 52.8 L h⁻1 over 120 hours. Our work unlocks a potent tool for efficient and sustainable plastic waste utilization.