Single atom catalysts (SACs) have played a significant role in heterogeneous catalysis fields, exhibiting the catalytic activity and stability. Especially, in formic acid synthesis by CO2 hydrogenation, carbon supported Ru SAC systems showed high stability as well as high activity. One of important SAC roles based on N-doped carbon supports prevents typical deactivation behaviors such as agglomeration and leaching over reductive conditions. However, because the carbon supporting materials suffers from the difficult fabrication of carbon particles for commerical use, it is necessary to find the catalytic SAC supporting metal oxide materials that is easily pelletized or extruded. To overcome this issue, we prepared N-doped TiO2 support materials to metalate Ru at various calcination temperature (MN–TiO2-Tcalc) and characterized structural and electronic properties of crystalline TiO2 and N dopant sites of prepared catalysts, identifying the two types of chemical state, i.e., substitutional N (Ns) and interstitial N (Ni) using NEXAFS and EXAFS. From the activity tests using Ru metalated MN-TiO2-Tcal catalysts, it was observed that the different catalytic activity and stability were correlated with the substitutional N structure and we showed the origins of the N structure with higher activity and stability in formate synthesis by CO2 hydrogenation through the DFT calculations.

N-doped TiO2 supported Ru SAC catalytic systems for formate synthesis by CO2 hydrogenation

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