Transition Metals (TMs) are ubiquitous materials employed in a myriad of industrially and technologically relevant fields. These range from energy storage devices , through drug release nanotechnologies , and to heterogeneous catalysis , to name a few. The interaction of carbon monoxide (CO) with catalytic TM surfaces has been extensively studied in the past due to its importance to chemical industries . The CO properties paved the way to its use as a probe molecule to obtain atomistic information on the studied surfaces upon CO adsorption . Besides its use as a probe molecule in the field of Surface Science, it is also used a reactant, e.g., in the Fischer-Tropsch (FT) process, generating hydrocarbons from CO:H2 mixtures , a key ingredient for the carbon circular economy when CO is generated from previously captured and dissociated carbon dioxide (CO2). Aside, CO is a sought product, for instance, through the reverse water gas shift reaction, where CO2 can be revalued by reacting with H2 to yield CO and H2O (CO2 + H2 → CO + H2O, ΔH r o = 41 kJ•mol -1 ) , with the concomitant environmental implications in the fight against global warming and climate change. Apart from these, the CO molecule can be a key intermediate, e.g. as in the course of CO2 hydrogenation towards methanol fuel, again key in making carbon economy circular . Thus, the interaction of CO with TM-based catalysts has gained importance as a way, not only to gain atomistic insights of the latter using CO as a probe molecule, but also as a crucial species in diverse processes of industrial and environmental relevance.