Gao Li, Zhong Xia, Liu Jie, Chen Junnan, Wang Ziru, Zhang Ying, Wang Deli, Shakeri Mozaffar, Zhang Xia, Zhang Bingsen
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, Liaoning, China.
School of Materials Science and Engineering, University of Science and Technology of China, Shenyang, 110016, Liaoning, China.
ChemSusChem. 2024 Oct 7;17(19):e202400598. doi: 10.1002/cssc.202400598. Epub 2024 Jun 4.
It has been known that plastics with undegradability and long half-times have caused serious environmental and ecological issues. Considering the devastating effects, the development of efficient plastic upcycling technologies with low energy consumption is absolutely imperative. Catalytic hydrogenolysis of single-use polyethylene over Ru-based catalysts to produce high-quality liquid fuel has been one of the current top priority strategies, but it is restricted by some tough challenges, such as the tendency towards methanation resulting from terminal C-C cleavage. Herein, we introduced Ru nanoparticles supported on hollow ZSM-5 zeolite (Ru/H-ZSM-5) for hydrocracking of high-density polyethylene (HDPE) under mild reaction conditions. The implication of experimental results is that the 1Ru/H-ZSM-5 (~1 wt % Ru) acted as an effective and reusable bifunctional catalyst providing higher conversion rate (82.53 %) and liquid fuel (C-C) yield (62.87 %). Detailed characterization demonstrated that the optimal performance in hydrocracking of PE could be attributed to the moderate acidity and appropriate positively charged Ru species resulting from the metal-zeolite interaction. This work proposes a promising catalyst for plastic upcycling and reveals its structure-performance relationship, which has guiding significance for catalyst design to improve the yield of high-value liquid fuels.
众所周知,具有不可降解性和长半衰期的塑料已引发严重的环境和生态问题。鉴于这些破坏性影响,开发低能耗的高效塑料升级循环技术势在必行。在钌基催化剂上对一次性聚乙烯进行催化氢解以生产高质量液体燃料一直是当前首要战略之一,但它受到一些严峻挑战的限制,例如末端碳 - 碳键断裂导致的甲烷化倾向。在此,我们引入了负载在中空ZSM - 5沸石上的钌纳米颗粒(Ru/H - ZSM - 5),用于在温和反应条件下对高密度聚乙烯(HDPE)进行加氢裂化。实验结果表明,1Ru/H - ZSM - 5(约1 wt%Ru)作为一种有效且可重复使用的双功能催化剂,提供了更高的转化率(82.53%)和液体燃料(C - C)产率(62.87%)。详细表征表明,PE加氢裂化的最佳性能可归因于适度的酸度以及由金属 - 沸石相互作用产生的适当带正电的钌物种。这项工作提出了一种有前景的塑料升级循环催化剂,并揭示了其结构 - 性能关系,这对催化剂设计以提高高价值液体燃料的产率具有指导意义。