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New technologies for the efficient utilization of fossil fuels are important to develop to reduce fossil fuel consumption and ameliorate the harmful effects on the global environment. Polymer electrolyte fuel cell (PEFC) systems are one of these technologies, which offer high power density and high total energy conversion efficiency. The PEFC can be operated at low temperature (ca. 80 °C), leading to easy start up and shut down, which is one of the main advantages, compared to other types of fuel cell such as solid oxide fuel cells. The PEFC produces electric energy via H2 oxidation. In the future, H2 could be produced from water electrolysis, although hydrogen-rich gas is presently obtained f rom fossil fuels. However, the hydrogen-rich gas contains a significant amount of CO which poisons the Pt catalysts on the anode. Therefore, the CO concentration must be reduced from ca. 10 % to 0.2-2 % by a water-gas shift reaction (WGS reaction, CO+H2O→CO2+H2) 1), and then to <100 ppm by preferential oxidation of CO in the presence of excess H2 (PROX, CO+1/2 O2→ CO2) 2),3). However, the PROX process is associated with oxidation of hydrogen in the presence of oxygen, leading to lower overall energy conversion efficiency for the PEFC. CO methanation (CO+3H2→ CH4+H2O) is another process of CO purification carried out in the presence of excess CO2. In 1970, Rehmat and Randhava suggested a concept of CO methanation for a fuel cell application5). Methanation of CO has the advantages that the reactants are already present for this reaction (CO and H2) in the reformed gas, and that the produced CH4 can be recycled as a heating fuel for the reforming unit. High selectivity is important for the removal of CO by methanation, or simultaneous CO2 methanation (CO2+4H2→ CH4+2H2O) and reverse water gas shift reaction (RWGS reaction, CO2+H2→ CO+H2O) will result in significant consumption of produced H2. Additionally, exothermic CO2 methanation carries the risk of runaway of the methanation reactor. Therefore, suitable catalysts must be developed to promote CO methanation at low temperatures and suppress CO2 methanation and RWGS reaction at high temperatures, leading to a wide operating temperature range for selective CO methanation. A great deal of effort has been made in studies of selective CO methanation in the presence of CO2 and H2O 80 Journal of the Japan Petroleum Institute, 61, (2), 80-86 (2018)

Degradation Factors of Ni/TiO<sub>2</sub> Catalysts for Selective CO Methanation: Effect of Loss of Residual Cl on Catalyst