Coordination-tuned Ru single-atom catalyst for efficient catalysis of CO2 to CH4 on RuBxN4-x@TiN (x=0–4)

Abstract

Creating useful chemicals or fuels from CO2 is one of the most promising ways to reach carbon neutral. In this work, through the formation of Lewis acid sites, a string of boron-atom-coordinated Ru single-atom catalysts (SACs), namely RuBxN4-x@TiN (x=0–4), were constructed, and their CO2 reduction reaction (CO2RR) was systematically studied. The results show that o-RuB2N2@TiN, p-RuB2N2@TiN, and RuB3N1@TiN are able to efficiently inhibit the competitive hydrogen evolution reaction (HER) and activate CO2, with a potential-determining step lower than 0.7 eV and high selectivity for CH4 generation. This work shows that the synergistic effect of B and Ru atoms are able to effectively improve the catalytic activity, which is expected to offer a possible tactic for the sensible creation of effective CO2RR catalysts.

Keywords

• TiN
• CO2 reduction
• Lewis acid sites
• Density functional theory
• Coordination-tuned