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

Abstract

AbstractRational 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.