Boosting Low‐Temperature CO2 Hydrogenation over Ni‐based Catalysts by Tuning Strong Metal‐Support Interactions

Rational design of low-cost and efficient transition-metal catalysts for low-temperature CO₂ activation is significant and poses great challenges. Herein, a strategy via regulating the local electron density of active sites is developed to boost CO₂ methanation that normally requires >350 °C for commercial Ni catalysts. An optimal Ni/ZrO₂ catalyst affords an excellent low-temperature performance hitherto, with a CO₂ conversion of 84.0 %, CH₄ selectivity of 98.6 % even at 230 °C and GHSV of 12,000 mL g^-1 h^-1 for 106 h, reflecting one of the best CO₂ methanation performance to date on Ni-based catalysts. Combined a series of in situ spectroscopic characterization studies reveal that re-constructing monoclinic-ZrO₂ supported Ni species with abundant oxygen vacancies can facilitate CO₂ activation, owing to the enhanced local electron density of Ni induced by the strong metal-support interactions. These findings might be of great aid for construction of robust catalysts with an enhanced performance for CO₂ emission abatement and beyond.