Upcycling polyolefins to methane-free liquid fuel by a Ru1-ZrO2 catalyst

IF 15.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Nature Communications Pub Date : 2025-03-21 DOI:10.1038/s41467-025-57998-x

Jicong Yan, Guanna Li, Zhanwu Lei, Xiaolu Yuan, Junting Li, Xiaoru Wang, Bo Wang, Fuping Tian, Tao Hu, Lei Huang, Yujia Ding, Xiaoke Xi, Feng Zhu, Shuo Zhang, Jiong Li, Yu Chen, Ruiguo Cao, Xiang Wang

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Abstract

Upcycling waste plastics into liquid fuels presents significant potential for advancing the circular economy but is hindered by poor selectivity and low-value methane byproduct formation. In this work, we report that atomic Ru-doped ZrO₂ can selectively convert 100 grams of post-consumer polyethylene and polypropylene, yielding 85 mL of liquid in a solvent-free hydrocracking. The liquid (C₅-C₂₀) comprises ~70% jet-fuel-ranged branched hydrocarbons (C₈-C₁₆), while the gas product is liquefied-petroleum-gas (C₃-C₆) without methane and ethane. We found that the atomic Ru dopant in the Ru-O-Zr moiety functionalizes its neighboring O atom, originally inert, to create a Brønsted acid site. This Brønsted acid site, rather than the atomic Ru dopant itself, selectively governs the internal C−C bond cleavage in polyolefins through a carbonium ion mechanism, thereby enhancing the yield of jet-fuel-ranged hydrocarbons and suppressing methane formation. This oxide modulation strategy provides a paradigm shift in catalyst design for hydrocracking waste plastics and holds potential for a broad spectrum of applications.

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用Ru1-ZrO2催化剂将聚烯烃升级为无甲烷液体燃料

将废塑料升级为液体燃料在推进循环经济方面具有巨大潜力，但由于选择性差和低价值甲烷副产品的形成而受到阻碍。在这项工作中，我们报告了原子钌掺杂ZrO2可以选择性地转化100克消费后的聚乙烯和聚丙烯，在无溶剂加氢裂化中产生85毫升液体。液体（C5-C20）含有~70%的喷气燃料范围的支链烃（C8-C16），而气体产品为液化石油气（C3-C6），不含甲烷和乙烷。我们发现Ru-O- zr部分中的Ru掺杂原子使其相邻的O原子功能化，从而产生了一个Brønsted的酸位。Brønsted酸位，而不是原子Ru掺杂剂本身，通过碳离子机制选择性地控制聚烯烃中内部C - C键的裂解，从而提高了喷气燃料烃类的产量，抑制了甲烷的形成。这种氧化物调制策略为加氢裂化废塑料的催化剂设计提供了一种范式转变，并具有广泛的应用潜力。

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来源期刊

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.