Optimizing low-temperature CO2 methanation through frustrated Lewis pairs on Ni/CeO2 catalysts

The promising realm of carbon dioxide (CO2) conversion offers a compelling avenue to advance environmental sustainability. This study introduces a novel approach by utilizing frustrated Lewis pairs (FLPs) for efficient lowtemperature CO2 methanation. Through a tailored ammonium bicarbonate (AB) precipitation method, we engineered Ni/CeO2 catalysts abundant in FLPs. Various morphologies, including aggregated flakes, broom -like structures, and irregular granules, were achieved by modulating the AB -to -cerium molar ratio. The distinctive broom -like Ni/(0.06AB)CeO2 catalyst, comprised of nanorods with abundant FLPs, exhibited outstanding lowtemperature CO2 methanation performance: 67.5 % CO2 conversion, 99.6 % CH4 selectivity, and 0.27 s-1 CO2 turnover frequency (TOFCO2) at 240 C-degrees, with excellent stability in a 100-h test at 300 C-degrees. Furthermore, leveraging in -situ DRIFTS and in -situ Raman techniques, and DFT study, we unraveled CO2 hydrogenation pathways and found a dual interplay of CO and formate pathways in the low -temperature methanation over Ni/(0.06AB)CeO2 catalyst.