Surface Coverage-Controlled C–C Coupling for Sustainable Formation of C1 and C2 Products

Growing energy needs and the eventual use of nonrenewable energy sources are resulting in the hasty release of carbon dioxide (CO2) and carbon monoxide (CO). The most effective and environmentally friendly option is the transformation of these hazardous gases into sustainable fuels. Subsequently, the central focus of this research is to explore the possibilities of CO(g) conversion into single- and multicarbon products such as methane, methanol, ethylene, and ethanol through an electrocatalytic CO reduction reaction (CORR). However, CO coverage over catalytic surfaces can impact CORR; this is why we explored the transition metal carbonitrides (TMCNs) under 25% CO coverage for C1 and C2 product formation by using density functional theory (DFT). During our observations, TaCN was found to be a highly promising surface for methanol and ethanol production at an onset potential of less than −0.50 V vs reversible hydrogen electrode (RHE). While WCN was identified as the most active catalyst for methane and ethanol formation at a potential less than −0.60 V vs RHE, further hydrogen evolution was not problematic for any TMCNs, while each slab was readily available for CORR. Overall, our predictions revealed that carbonitrides can be employed for sustainable fuel production at the lowest possible potentials, paving the way for their experimental implementation in pursuit of a greener future.