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In the context of large-scale utilisation of renewable energy sources, mitigating the fluctuating nature of renewable power generation is crucial. Synthetic natural gas, produced from CO2 and H2 derived from water electrolysis, is considered a potential energy carrier to store excess electrical energy. The viability of this “power-to-gas” concept will, amongst others, depend on active and inexpensive catalytic systems. Typical CO2 methanation catalysts are supported transition and noble metals. Understanding the mechanism, periodic trends, structure sensitivity and support effects of the Sabatier reaction is essential to develop better methanation catalysts. In this chapter, recent advances in understanding and controlling the performance of methane production from CO2 will be reviewed by examining key mechanistic proposals and structure–activity relationships.

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