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India

Name	Rajesh BINIWALE
Position	Scientist Air Pollution Control Division, National Environmental Engineering Research Institute
Japanese Advisor	Masaru ICHIKAWA Professor,Hokkaido University

Catalysis in Octane Reforming and Cyclohexane Dehydrogenation Reactions using Plasma-Spray Pulsed Reactors and their Thermographic Reaction Analysis for Hydrogen Production, Storage and Supply

Catalytic processes for hydrogen production, storage & supply, and utilization are being considered as most important issues for application of clean energy resources. In present study two important aspects namely; hydrogen production and, storage & supply are addressed. Hydrogen production was carried out via reforming of iso-octane. Catalytic dehydrogenation of cyclohexane was studied for hydrogen storage and supply application. Novel reactors having spray-pulsed mode injection of liquid reactant have been used for generating higher concentration of reactant on catalysts surface under gas-liquid multiphase and maintain higher surface temperature to facilitate the endothermic reactions. Further in case of iso-octane reforming the higher energy requirement for reforming was supplied by use of non-thermal plasma and by maintaining the lower reaction temperatures.
Iso-octane was used in this study to simulate the reforming of gasoline under autothermal conditions. A steam/carbon ratio equal to 1 and an equivalence ratio equal to 0.32 was used for reforming at temperatures of 600 and 700°C on Ni-Mn, Ni-W and Rh-Ce catalysts supported on alumina mesh. A novel spray-pulsed reactor for providing atomized iso-octane in pulses was used to create alternate wet and dry conditions for improving the catalyst reactant contact which resulted in enhanced hydrogen production rates. The maximum hydrogen yield obtained is 4 moles of hydrogen per mole of iso-octane. Based on the product analysis optimized condition for higher hydrogen production and high H2/CO ratio has been deduced. Further, the effect of non-thermal plasma in combination with catalyst on reaction was tested under spray-pulse injection of iso-octane for energy efficient system. Plasma catalytic hybrid system results into higher activity at particularly gas-liquid multiphase conditions.

Figure 1: Experimental setup for Plasma-Spray Pulsed Reactor

Cycloalkanes can be used for efficient storage and supply of hydrogen both on weight (6-8 wt%) and volume basis (60 to 65 kg-H2/m³)without any contamination of other gases such as CO. Dehydrogenation of cyclohexane over Pt/alumite and Pt/activated carbon cloth catalysts was carried out for hydrogen storage and supply to fuel cell applications. Unsteady state was created using spray pulsed injection of cyclohexane to facilitate the endothermic reaction to occur efficiently. Higher temperature of the catalysts surface is more favorable for this reaction, thus the heat transfer phenomena and temperature profile under alternate wet and dry conditions created using spray pulsed injection becomes important. IR thermography was used for monitoring of temperature profile of the catalyst surface simultaneously with product analysis. The heat flux from the plate type heater to the catalyst was estimated (10-15 kW/m²) using a rapid temperature recording and thermocouple arrangement. The analysis of temperature profiles, reaction products over two different supports namely activated carbon cloth and alumite reveals that the more conductive support such as alumite is more suitable for dehydrogenation of cyclohexane.

With the specific interest to use non-noble metal catalysts or to minimize the use of Pt in catalysts, dehydrogenation of cyclohexane to benzene was carried out over Ni supported on activated carbon cloth (Ni/ACC). A synergistic effect was observed in the case of the promoted catalysts.
Further, supported perovskite catalysts with higher surface areas have been synthesized and used for emission reduction particularly may be formed during use of fossil fuel combustion for providing energy to the reforming reactions. The results reported in this study would be beneficial for advancement in hydrogen production and; storage and supply for fuel cell applications.

Asian Program Division
Japan Society for the Promotion of Science (JSPS)
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