Synthesıs, Characterızatıon And Reactıon Studıes On Cerıum Oxıde, Alumına And Sılıcate Supported Iron, Nıkel And Cobalt Incorporated Catalysts For Hydrogen Productıon


Thesis Type: Postgraduate

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

Approval Date: 2015

Student: İBRAHİM ETHEM DOĞANAY

Supervisor: DİLEK VARIŞLI

Abstract:

Nowadays, ammonia has become an important raw material for the production of COx free hydrogen which is especially necessary for PEM fuel cells. In this thesis work, with the aim of producing hydrogen from ammonia at high yield, cerium oxide (CeO2), alumina (Al2O3) and silicate (SiO2) supported catalysts with the incorporation of different metals, namely, iron, nikel and cobalt, were prepared. Wet impregnation procedure was used in the synthesis of the catalysts and the weight ratio of metal precursor to support material was changed between 0.05 and 1.0. Physical and structural properties of catalysts were determined by different techniques such as Nitrogen Physisorption, XRD, SEM-EDS. The catalytic activities of catalysts on ammonia decomposition reaction to produce hydrogen were tested in a fixed bed flow reactor using 0.1 g of fresh catalyst in a temperature range of 400 to 700 oC under the continous flow of pure ammonia with a rate of 60 ml/min While pure cerium oxide which was used as a support material for the synthesized catalysts as well, gave 70 % ammonia conversion at 600oC, iron supported ones gave ammonia conversion over 90%. Under the same reaction conditions overall conversion could be achieved over Co@CeO2 type catalysts, which were prepared by using cobalt nitrate, and Ni@CeO2 type catalysts, which were prepared by using nikel chloride.Among the alumina supported catalysts, iron incorporated ones with a loading ratio of 0,4 and above, gave approximatelly 90 % ammonia conversion. In the case of nikel and cobalt incorporated alumina supported catalysts an optimum value for metal loading was observed to obtain the highest activity. Catalysts namely, Ni@Al2O3(0,2) and Co@Al2O3(0,4) gave overall conversion at a reaction temperature of 600oC. Among the silicate supported nikel incorporated catalysts Ni@SiO2(0,4) gave the highest activity under the same reaction condition. Results of the experiments indicated that parameters such as metal loading ratio, metal dispersion, surface area of catalyst and metal- support interaction had great affects on the actvities of cerium oxide, alumina and silicate supported metal incorporated catalysts for hydrogen production from ammonia.