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Photothermal CO2 reduction is an efficient and sustainable catalytic path for CO2 treatment. Here, we successfully fabricated a novel series of Ni-based catalysts (Ni-x) via H2 reduction of NiAl-layered double hydroxide nanosheets at temperatures (x) ranging from 300 to 600 ℃. With the increase of the reduction temperature, the methane generation rate of the Ni-x catalyst for photothermal CO2 hydrogenation gradually increased under ultraviolet-visible-infrared (UV–vis–IR) irradiation in a flow-type system. The Ni-600 catalyst showed a CO2 conversion of 78.4%, offering a CH4 production rate of 278.8 mmol·g–1·h–1, with near 100% selectivity and 100 h long-term stability. Detailed characterization analyses showed metallic Ni nanoparticles supported on amorphous alumina are the catalytically active phase for CO2 methanation. This study provides a possibility for large-scale conversion and utilization of CO2 from a sustainable perspective.
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