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Structure-activity relationship in hydrogenolysis of polyolefins over Ru/support catalysts
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-08-18 , DOI: 10.1016/j.apcatb.2022.121870
Masazumi Tamura , Shuhei Miyaoka , Yosuke Nakaji , Mifumi Tanji , Shogo Kumagai , Yoshinao Nakagawa , Toshiaki Yoshioka , Keiichi Tomishige

We scrutinized the effect of supports (types and calcination temperatures) in Ru/support catalysts in the hydrogenolysis of low-density polyethylene and found that zirconia-supported Ru (Ru/ZrO2) with high-temperature (1073 K) calcined ZrO2 was an effective and reusable catalyst, showing about 3-fold higher activity on catalyst amount basis than the previously reported Ru/CeO2 catalyst with similar selectivites. The catalyst was applicable to the reactions of various polyolefins including high-density polyethylene and polypropylene. Experimental studies and catalyst characterizations such as TPR, XRD, TEM and XAS with various Ru/ZrO2 and reference catalysts such as Ru/CeO2, Ru/SiO2 and Ru/γ-Al2O3 showed good correlations between the Ru particle sizes and catalytic performance in Ru catalysts except for Ru/γ-Al2O3: The catalyst with a moderate size of ~2.5 nm Ru particles provided the highest conversion. The activity per surface Ru metal was higher at larger Ru particle sizes. The selectivity to cheap gas products was low at middle to small Ru particle sizes (1~7 nm), but high at large Ru particles (>7 nm).



中文翻译:

Ru/载体催化剂上聚烯烃氢解的构效关系

我们仔细研究了低密度聚乙烯氢解中 Ru/载体催化剂中载体(类型和煅烧温度)的影响,发现氧化锆负载的 Ru (Ru/ZrO 2 ) 与高温 (1073  K) 煅烧的 ZrO 2是一种有效且可重复使用的催化剂,以催化剂量计,其活性比先前报道的具有相似选择性的 Ru/CeO 2催化剂高约 3 倍。该催化剂适用于高密度聚乙烯、聚丙烯等多种聚烯烃的反应。实验研究和催化剂表征,例如 TPR、XRD、TEM 和 XAS,使用各种 Ru/ZrO 2和参考催化剂,例如 Ru/CeO 2、Ru/SiO 2和Ru/γ-Al 2 O 3在Ru催化剂中除了Ru/γ-Al 2 O 3之外,Ru颗粒尺寸和催化性能之间表现出良好的相关性:具有~2.5  nm的中等尺寸Ru颗粒的催化剂提供了最高的转化率. 在较大的Ru粒径下,每个表面Ru金属的活性较高。对廉价气体产品的选择性在中小Ru颗粒(1~7  nm)时较低,但在大Ru颗粒(>7  nm)时选择性较高。

更新日期:2022-08-18
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