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

Abstract Rational design of low‐cost and efficient transition‐metal catalysts for low‐temperature CO 2 activation is significant and poses great challenges. Herein, a strategy via regulating the local electron density of active sites is developed to boost CO 2 methanation that normally requires >350 °C for commercial Ni catalysts. An optimal Ni/ZrO 2 catalyst affords an excellent low‐temperature performance hitherto, with a CO 2 conversion of 84.0 %, CH 4 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 CO 2 methanation performance to date on Ni‐based catalysts. Combined a series of in situ spectroscopic characterization studies reveal that re‐constructing monoclinic ‐ZrO 2 supported Ni species with abundant oxygen vacancies can facilitate CO 2 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 CO 2 emission abatement and beyond.