Synthesis and characterization of ruthenium based silicate catalysts and studies on hydrogen synthesis


Thesis Type: Postgraduate

Institution Of The Thesis: Gazi Üniversitesi, Fen Bilimleri Enstitüsü, Turkey

Approval Date: 2012

Student: EKREM EMRE ELVERİŞLİ

Supervisor: DİLEK VARIŞLI

Abstract:

Hydrogen is consedered being a clean alternative energy source due to its superior properties. In this study Ruthenium-silicate based nanocomposite structured catalysts were prepared by direct hydrothermal synthesis procedure, characterized TGA-DTA, XRD, N2 Physisorption, HRTEM, SEM-EDX techniques and their activites were tested in fixed bed flow reactor. In the preparation of the catalysts, different parameters such as different silicate sources, different ruthenium loading amount and the addition of promoter were investigated. Distribution of active metals throughout the catalysts structure, high surface area and usage of KOH as a promoter enhanced the activities of catalysts for ammonia decomposition reaction. Experiments carried out under the high flow rate of ammonia (300ml/min) presented that 86% ammonia conversion was obtained at 500oC over the catalyst having Ru/Si molar ratio of 0.060. Using promoter in the prepation of catalyst enhanced the activity of the catalyst especially for the one prepared at low ruthenium loading. While the catalyst that was prepared without promoter at a Ru/Si molar ratio of 0.10 gave negligible activity at 500oC, the one prepared with promoter gave 33% conversion at 500oC and 73% at 600oC. Experiments were also repeated with lower feed flow rate values of ammonia such as 60 ml/min and 5 ml/min. It was seen that catalysts prepared with promoter at a Ru/Si molar ratio of 0.010 gave conversion values over 80% at 400oC under the feed flow rate of 5ml/min. Bimetallic catalysts that contained nickel and ruthenium gave 91% conversion at 600oC under the high ammonia feed flow rate (300ml/min). Direct hydrothermal synthesis procedure was also applied for the synthesis of Rhodium-silicate based catalysts and results of activity studies presented that the catalyst having Rh/Si molar ratio of 0.015 gave conversion over 70% at 600oC under 300ml/min of ammonia flow.