The CO hydrogenation on single-crystal ruthenium catalysts has been studied utilizing an elevated-pressure micro-reactor and high resolution electron energy loss spectroscopy (HREELS). It is found that carbonaceous deposits identified following CO hydrogenation are essentially identical to those observed in the study of methane decomposition. Three distinct forms of carbonaceous intermediates are identified; these are methylidyne (CH), vinylidene (CCH2), and graphitic carbonaceous species.