Zieliński Michał, Janiszewska Ewa, Drewniak Adrianna, Pietrowski Mariusz
Faculty of Chemistry, Adam Mickiewicz University, Uniwersytetu Poznańskiego 8, 61-614 Poznań, Poland.
Molecules. 2023 Aug 31;28(17):6376. doi: 10.3390/molecules28176376.
This study focuses on the catalytic properties of ruthenium catalysts supported on modified silicalite-1 (with an MFI structure). By post-synthesis modification of silicalite-1 with solutions of alkali metal compound, a novel and cost-effective method was discovered to create basic centers on the surface of silicalite-1 supports. The modification not only affected the basicity of the supports but also their porosity. The influence of the type of alkali solution (KOH or NaOH) and its concentration (0.1 M or 1.0 M) on both the basicity and porosity was investigated. The modified silicalite-1 materials were employed as supports for ruthenium catalysts (1 wt.% Ru) and evaluated for their CO methanation activity. The results were compared with the hydrogenation performance of ruthenium catalysts supported on unmodified silicalite-1. Characterization of the supports and catalysts was conducted using techniques such as BET, XRD, FT-IR, ICP-OES, TPR-H, H chemisorption, TPD-CO, SEM, and TEM. Remarkably, the catalytic activity of ruthenium supported on silicalite-1 treated with 1.0 M NaOH (exhibiting selectivity toward methane above 90% in a reaction temperature range of 250-450 °C) outperformed both unmodified and KOH-modified silicalite-1 supported Ru catalysts.
本研究聚焦于负载在改性硅沸石-1(具有MFI结构)上的钌催化剂的催化性能。通过用碱金属化合物溶液对硅沸石-1进行后合成改性,发现了一种新颖且经济高效的方法来在硅沸石-1载体表面产生碱性中心。该改性不仅影响了载体的碱性,还影响了其孔隙率。研究了碱溶液类型(KOH或NaOH)及其浓度(0.1 M或1.0 M)对碱性和孔隙率的影响。将改性后的硅沸石-1材料用作钌催化剂(1 wt.% Ru)的载体,并对其CO甲烷化活性进行评估。将结果与负载在未改性硅沸石-1上的钌催化剂的氢化性能进行比较。使用BET、XRD、FT-IR、ICP-OES、TPR-H、H化学吸附、TPD-CO、SEM和TEM等技术对载体和催化剂进行表征。值得注意的是,负载在1.0 M NaOH处理的硅沸石-1上的钌的催化活性(在250 - 450 °C的反应温度范围内对甲烷的选择性高于90%)优于未改性和KOH改性的负载钌的硅沸石-1催化剂。