Scholarlink

<p>Polyolefin waste presents a major upcycling challenge because of its chemical inertness. Ruthenium catalysts are highly active for polyethylene hydrogenolysis, but often overproduce methane and linear alkanes and show limited substrate scope. Here we establish a mechanistic framework showing that the interplay between Ru nuclearity, valence, and support acidity governs the selectivity in Ru/NbO<sub>x</sub>-catalyzed polyolefin hydroconversion. Metallic Ru nanoparticles activate both C-H and C-C bonds and favor hydrogenolysis, whereas atomically dispersed Ru species, together with hydrogen spillover-generated Nb-OH sites, enable C-H activation and Brønsted acid-assisted hydrocracking. Methane originates primarily from hydrogenolysis on extended metallic Ru domains and is minimized by controlling Ru ensemble size or shifting the reaction toward hydrocracking. Accordingly, Ru/NbO<sub>x</sub>-600 fully converts polyethylene to 93.1% C<sub>5-35</sub> linear alkanes, while Ru/NbO<sub>x</sub>-300 hydrocracks polypropylene at 1731 g<sub>PP</sub>·g<sub>Ru</sub><sup>-1</sup>·h<sup>-1</sup> with 90.6% C<sub>5-20</sub> branched liquid fuel selectivity. This work establishes design principles of Ru catalysts for selective, efficient plastic upcycling.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Nuclearity-dependent design principles of ruthenium catalysts for selective hydroconversion of diverse polyolefins

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年4月24日

查看全文
  • Jie Sun,
  • Yan Mei,
  • Xiaobing Ren,
  • Wei Cao,
  • Jiuxuan Zhang,
  • Zhengyan Qu,
  • Feng Zeng,
  • Hong Jiang,
  • Zhenchen Tang,
  • Rizhi Chen

摘要

Polyolefin waste presents a major upcycling challenge because of its chemical inertness. Ruthenium catalysts are highly active for polyethylene hydrogenolysis, but often overproduce methane and linear alkanes and show limited substrate scope. Here we establish a mechanistic framework showing that the interplay between Ru nuclearity, valence, and support acidity governs the selectivity in Ru/NbOx-catalyzed polyolefin hydroconversion. Metallic Ru nanoparticles activate both C-H and C-C bonds and favor hydrogenolysis, whereas atomically dispersed Ru species, together with hydrogen spillover-generated Nb-OH sites, enable C-H activation and Brønsted acid-assisted hydrocracking. Methane originates primarily from hydrogenolysis on extended metallic Ru domains and is minimized by controlling Ru ensemble size or shifting the reaction toward hydrocracking. Accordingly, Ru/NbOx-600 fully converts polyethylene to 93.1% C5-35 linear alkanes, while Ru/NbOx-300 hydrocracks polypropylene at 1731 gPP·gRu-1·h-1 with 90.6% C5-20 branched liquid fuel selectivity. This work establishes design principles of Ru catalysts for selective, efficient plastic upcycling.