Decomposition and regeneration of methane in the absence and the presence of a hydrogen-absorbing alloy CaNi5 Original Research Article

Suitable catalysts for the decomposition of methane into carbon and hydrogen and for the regeneration of methane by hydrogenation of the carbon have been looked for in a series of transition metals and precious metals supported on various carriers. The most active catalyst for both reactions was Ni/SiO2. The carbon formed on this catalyst was thermodynamically less stable than graphite. The different rate equations for the decomposition of methane obtained for the fresh and carbon deposited Ni/SiO2 suggest that the rate-determining steps are different for the two catalysts. The highest number of carbon atoms deposited per one Ni atom was 31 at 773 K. However, the number of methane molecules recovered easily at 773 K was limited to 1.5 per Ni atom. A physical mixture of Ni/SiO2 and CaNi5, a hydrogen-absorbing alloy, enhanced the decomposition rate of methane, enabling the complete conversion of methane at 773 K beyond the thermodynamic limitation. The presence of CaNi5 at 273 K separated from the catalyst in a reaction system further enhanced the decomposition of methane due to an increased hydrogen-absorbing capacity of the CaNi5 at low temperatures. The carbon deposited on Ni/SiO2 in this case was reactive to be hydrogenated back to methane at 773 K, giving an average 7.5 CH4 molecules per one Ni atom