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CoMn 2 O 4 spinel sorbent was applied to remove Hg 0 in coalderived syngas. The impacts of syngas components, including H 2 S, H 2 , CO, HCl, and H 2 O, on Hg 0 abatement were examined. Moreover, the Hg 0 removal mechanism over the CoMn 2 O 4 surface was elucidated in detail by combining experiments and density functional theory (DFT) calculations. About 90% Hg 0 abatement was obtained using CoMn 2 O 4 sorbent in 40−200 °C under syngas atmosphere. H 2 S could adsorb and generate active sulfur upon CoMn 2 O 4 and, hence, played the most important role in Hg 0 elimination. HCl also facilitated Hg 0 capture by producing reactive chlorine compounds. Under N 2 atmosphere, H 2 , CO, and H 2 O played an inhibitory effect on Hg 0 removal, but they did not affect Hg 0 removal in the presence of H 2 S. Based on the experimental and DFT results, the Langmuir−Hinshlwood mechanism, where chemically adsorbed mercury interacts with surface sulfur from H 2 S dissociation, is responsible for the reaction between Hg 0 and H 2 S over CoMn 2 O 4 . After Hg 0 removal, HgS was formed and bonded to CoMn 2 O 4 sorbent, which was certified using TPD and XPS analyses.