In situ Doping Coupling With Vacancy Regulation Induced Strong Metal‐Support Interaction in Ni/CaTiO<sub>3</sub> to Boost Supercharged Photothermal CO<sub>2</sub> Methanation

Authors: Zhimin Yuan, Baokun Zhang, Xianglin Zhu, Shenghua Wang, Wei Sun, Baibiao Huang, Zaiyong Jiang, Ying Dai, Zheng Wang, Wei Wei, Xishi Tai, Ya‐Qian Lan

Published: 2025-03-12

DOI: 10.1002/adfm.202503531

Source: Full article


Abstract

AbstractThe “Solar Sabatier” reaction has emerged as a promising sustainable method for the CO2 hydrogenation. The development of advanced metal‐support catalysts based on Strong Metal‐Support Interaction (SMSI) offers significant advantages in the activation of CO2 and the regulation of selectivity. Herein, a novel composite Ni/CaTiO3 catalyst consisting of Ni and Ni‐doped CaTiO3 is synthesized and utilized in the CO2 methanation. A noteworthy finding is that the incorporation of Ni into the CaTiO3 matrix is instrumental in the formation of oxygen vacancies and the establishment of SMSI between Ni and CaTiO3. The enhanced SMSI resulting from the surface‐doped Ni atoms not only facilitated effective interface contact between metallic Ni and the CaTiO3 surface but also significantly improved the migration efficiency of hydrogen atoms reduced the reaction barrier for CO2 methanation and optimized the rate‐limiting step, all of which are advantageous for the CO2 methanation. Consequently, the optimized catalysts exhibited extraordinary performance, achieving a CO2 conversion rate of 87.77%, CH4 generation rate of 3.12 mol gNi−1 h−1, and ≈100% CH4 selectivity under ambient pressure conditions. This investigation lays the groundwork for the design of highly active “Solar Sabatier” catalysts and offers a novel understanding of the mechanisms underlying effective SMSI.