摘要
Nickle-based catalysts are commonly used for CO_(2)methanation.However,there is still potential to improve their catalytic performanc under mild conditions.In this study,we synthesized a series of Ru-Ni-Al catalysts from Ru-doped NiAl-hydrotalcite using a hydrotherma method.The Ru-Ni-Al catalyst demonstrated much higher activity for CO_(2)methanation than the Ni-Al catalyst that did not have Ru doping Both experimental results and theoretical calculations indicate that the enhanced performance of the Ru-Ni-Al catalyst is related to electroni interactions between nickel(Ni)and ruthenium(Ru).The Ru sites transfer electrons to the Ni sites,increasing the local electron density of Ni which enhances the adsorption and activation of H_(2).Furthermore,the Ru-Ni metal interface sites improve the adsorption and activation of CO_(2)In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy(DRIFTS)analysis indicates that adjusting the electronic structure of N sites can accelerate the production of intermediates HCOO^(*),while Ru-Ni intermetallic interface sites can directly dissociate CO_(2)into CO^(*).In addition,CO_(2)methanation on the Ru-Ni-Al catalyst follows HCOO^(*)-and CO^(*)-mediated pathways.This study underscores the potential fo enhancing CO_(2)methanation performance by modulating the electronic structure of Ni sites.
基金
support from the National Natural Science Foundation of China(22278006)
Open Project Fund from Guangdong Provincial Key Laboratory of Materials and Technology for Energy Conversion,Guangdong Technion-Israel Institute of Technology(MATEC2024KF009)
Open Research Fund of State Key Laboratory of Mesoscience and Engineering(MESO-23-D13)。
