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<p>Assessing the sustainability of plastic chemical recycling requires realistic feedstocks and catalysts designed within sustainability-led frameworks (Plastic-to-X). We link catalyst design and systems analysis to study hydrogenolysis of high-density polyethylene (virgin and bottle caps; <i>M</i><sub>w</sub> = 100–200 kDa). We report&#xa0;Ru–Ni alloy nanoparticles (3–4 nm) supported on titania that yield up to 55% liquid C<sub>6</sub>–C<sub>45</sub> products under optimized conditions, whereas monometallic Ru produces virtually no liquids&#xa0; <i>Operando</i> spectroscopy and simulations reveal structure sensitivity: backbone scission follows dehydrogenation and hydrogenation cycles at defective alloy sites formed in situ. Integrating these mechanistic insights with life cycle and techno-economic analyses indicates profitable processing of plastic caps over the optimal catalyst (2.5 wt% Ru, 5 wt% Ni) with substantially lower CO<sub>2</sub> emissions even when using green H<sub>2</sub>. Furthermore, within the Plastic-to-X framework, we identify a minimum average chain length threshold of C<sub>11</sub> for product distributions as a &#xa0;critical design&#xa0; metric to reconcile environmental and economic objectives.</p>

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Polyethylene hydrogenolysis to liquid products over bimetallic catalysts with favorable environmental footprint and economics

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年11月10日

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  • Iris Nogueroles-Langa,
  • Yuzhen Ge,
  • Cecilia Salah,
  • Shibashish D. Jaydev,
  • Jordi Morales-Vidal,
  • Pol S. Berman,
  • Henrik Eliasson,
  • Rolf Erni,
  • Gonzalo Guillén-Gosálbez,
  • Núria López,
  • Antonio J. Martín,
  • Javier Pérez-Ramírez

摘要

Assessing the sustainability of plastic chemical recycling requires realistic feedstocks and catalysts designed within sustainability-led frameworks (Plastic-to-X). We link catalyst design and systems analysis to study hydrogenolysis of high-density polyethylene (virgin and bottle caps; Mw = 100–200 kDa). We report Ru–Ni alloy nanoparticles (3–4 nm) supported on titania that yield up to 55% liquid C6–C45 products under optimized conditions, whereas monometallic Ru produces virtually no liquids  Operando spectroscopy and simulations reveal structure sensitivity: backbone scission follows dehydrogenation and hydrogenation cycles at defective alloy sites formed in situ. Integrating these mechanistic insights with life cycle and techno-economic analyses indicates profitable processing of plastic caps over the optimal catalyst (2.5 wt% Ru, 5 wt% Ni) with substantially lower CO2 emissions even when using green H2. Furthermore, within the Plastic-to-X framework, we identify a minimum average chain length threshold of C11 for product distributions as a  critical design  metric to reconcile environmental and economic objectives.