Power-toGas (PtG) is an emerging grid-scale energy storage technology by which the surplus renewable electricity and captured CO2 are converted to synthetic natural gas as an energy carrier. In short, the off-grid, surplus electricity from renewable power sources such as wind and solar farms is utilized to electrolyze water via Solid-Oxide-Cell, and the generated hydrogen is then combined with CO2 through the Sabatier process to produce methane. The transportation of methane is mature and energy-efficient within the existing natural gas pipeline or town gas network. Additionally, it would be ideal to make use of the reverse function of SOEC, the Solid-Oxide-Fuel-Cell, to generate electricity when the grid is short of power. The electricity generation is important to lower the levelized cost of the energy stored in the system. On the other hand, the CO2 methanation (CO2 + 4H2 = CH4 + H2O) is one of the crucial steps in the PtG technology. It utilizes the existing natural gas infrastructure to store and transport the renewable energy in a largescale and long-distance. However, the strong exothermicity of the methanation process remains one of the major challenges for the scale-up of the technology, especially when the feedstocks are I also want to express my thank to my co-supervisor, Professor Wang Xin for his good advises on the aspect of chemical reaction engineering during our meetings and discussion. I truly appreciate the useful guidance on paper writing and critical thinking skills from my TAC member Professor Su Haibin. Without the scholarship support from my school, Nanyang Technological University, Interdisciplinary Graduate School, I couldn't have the chance and courage to pursue the degree. I would like to thank the university for providing the funding and the great environment for my study. Last but not least I would like to thank my wife and my parents for the spiritual support every day.