Ruthenium-catalyzed “open-loop” recycling of polyethylene via tandem isomerization-metathesis (ISOMET)†

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2024-09-30 DOI:10.1039/d4gc03912b

Vajk Farkas , Pascal Albrecht , Ádám Erdélyi , Márton Nagyházi , Beatrix Csutorás , Gábor Turczel , Norbert Miskolczi , Janka Bobek-Nagy , Ole Osterthun , Jürgen Klankermayer , Robert Tuba

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Abstract

As a model of a chemical upcycling process, we have developed a single-metal homogeneous catalytic system to break down persistent polyethylene waste into valuable chemical intermediates. This could ultimately be used to produce important chemical products, including environmentally friendly, biodegradable plastics. In the first step, a slow pyrolysis of polyolefin waste yields oils, containing long-chain olefins as the major components. Then, for the next transformation step, tailored bicyclic (alkyl)(amino)carbene (BICAAC)-Ru olefin metathesis catalysts were used in combination with an alkene isomerization catalyst (RuHCl(CO)(PPh₃)₃) for the transformation of the pyrolysis oil to propylene via isomerization-metathesis (ISOMET) reaction in ethylene atmosphere. Eventually, translation of the highly efficient single-metal catalyst system enabled ISOMET reaction to a 900 mL reactor setup and repetitive batch experiments could prove the long-term stability of the catalyst system and the highest total turnover number (tTON = 2788 mol propylene per mol olefin metathesis catalyst) reported so far using post-consumer polyethylene waste feedstock.

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钌催化的串联异构化-甲基化聚乙烯 "开环 "循环（ISOMET）

作为化学升级再循环工艺的典范，我们开发了一种单金属均相催化系统，可将持久性聚乙烯废料分解为有价值的化学中间体。这最终可用于生产重要的化学产品，包括环保型生物降解塑料。第一步，对聚烯烃废料进行缓慢热解，产生油类，主要成分是长链烯烃。然后，在下一个转化步骤中，将定制的双环（烷基）（氨基）碳烯（BICAAC）-Ru 烯烃偏聚催化剂与烯烃异构化催化剂（RuHCl(CO)(PPh3)3）结合使用，在乙烯气氛中通过异构化-偏聚（ISOMET）反应将热解油转化为丙烯。最终，高效单金属催化剂系统将 ISOMET 反应转化为 900 mL 反应器装置，重复批量实验证明了催化剂系统的长期稳定性，以及迄今为止所报道的使用消费后聚乙烯废料原料的最高总周转次数（tTON = 2788 摩尔丙烯/摩尔烯烃偏聚催化剂）。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.