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CO2 is the main component of greenhouse gases and also an important carbon source. The hydrogenation of CO2 to methane using Ni‐based catalysts can not only alleviate CO2 emissions but also obtain useful fuels. However, Ni‐based catalysts face one major problem of the sintering of Ni nanoparticles in the process of CO2 methanation. Thus, this work has synthesized a series of efficient and robust nickel silicate catalysts (NiPS−X) with different nickel content derived from nickel phyllosilicate by the hydrothermal method. It was found that the Ni loading plays a critical role in the structure and catalytic performance of the NiPS−X catalysts. The catalytic performance gradually increases with the increase of Ni loading. In particular, the highly dispersed NiPS‐1.6 catalyst with a high Ni loading of 34.3 wt% could obtain the CO2 conversion greater than 80%, and the methane selectivity was close to 100% for 48 h at 330 °C and the GHSV of 40,000 mL g−1 h−1. The excellent catalytic property can be assigned to the high dispersion of Ni nanoparticles and the strong interaction between the active component and the carrier, which is derived from a unique layered silicate structure with lots of nickel phyllosilicate and a large number of Lewis acid sites.

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