Low-Temperature CO2 Methanation over CeO2-Supported Ru Single Atoms, Nanoclusters, and Nanoparticles Competitively Tuned by Strong Metal–Support Interactions and H-Spillover Effect

Abstract

CO2 hydrogenation for the acquisition of value-added chemicals is an economical means to deal with the CO2-relevant environmental problems, among which CO2 reduction to CH4 is an excellent model reaction for investigating the initial steps of CO2 hydrogenation. For the supported catalysts commonly used in such reactions, the tailoring of the interfacial effect between metal centers and supporting materials so as to obtain superior low-temperature CO2 methanation performance is a significant but challenging subject. In this work, we altered the size regimes of the Ru deposits in Ru/CeO2 assemblies and uncovered the competitive relationship between the strong metal–support interactions (SMSI) and the H-spillover effect in determining the methanation activities by some ex situ and in situ spectroscopic techniques coupled with density functional theory (DFT) calculations. For CeO2 nanowire supported single Ru atoms, Ru nanoclusters (ca. 1.2 nm in size), and large Ru nanoparticles (ca. 4.0 nm in size), the nan...