Thermally cured nickel-based catalysts enabling high-activity plasma-assisted CO₂ hydrogenation

Global warming and the energy transition have intensified the demand for sustainable CO₂ utilization. Herein, we report a thermal-curing strategy for synthesizing highly efficient Nickel-based catalysts that enable low-temperature CO₂ methanation via both plasma-catalytic and thermocatalytic pathways. The optimized 10Ni/ZrO₂-50 nm catalyst achieves outstanding plasma-assisted performance, delivering up to 94.4% CO₂ conversion and 99% CH₄ selectivity at merely 25 W, alongside superior stability (240 h) and nearly complete CH₄ selectivity. Remarkably, in-situ plasma treatment alone effectively reduces surface Ni²⁺ species to metallic Ni⁰ even at room temperature, eliminating external heating requirements and significantly enhancing catalytic activity. Comprehensive characterization confirms that plasma exposure modulates metal-support interactions and surface oxygen species, thereby facilitating CO₂ activation via intermediates including surface-adsorbed carbonates, bicarbonate, formate, and carbon monoxide. This work demonstrates a scalable, energy-efficient route integrating catalyst design and plasma activation for sustainable CO₂ conversion toward carbon-neutral fuel synthesis.