The CO oxidation mechanisms over three different MnN-doped graphene (MnNC: MnNC-hex, MnNC-opp, MnNC-pen) structures were investigated through first-principles calculations. The vacancy in graphene can strongly stabilize Mn atoms and make them positively charged, which promotes O activation and weakens CO adsorption. Hence, CO oxidation activity is enhanced and the catalyst is prevented from being poisoned. CO oxidation reaction (COOR) on MnNC along the Eley-Rideal (ER) mechanism and the Langmuir-Hinshelwood (LH) mechanism will leave one O atom on the Mn atom, which is difficult to react with isolated CO. COOR on MnNC-opp along the ER mechanism and termolecular Eley-Rideal (TER) mechanism need overcome low energy barriers in the rate limiting step (RLS), which are 0.544 and 0.342 eV, respectively. The oxidation of CO along TER mechanism on MnNC-opp is the best reaction pathway with smallest energy barrier. Therefore, the MnNC-opp is an efficient catalysis and this study has a guiding role in designing effective catalyst for CO oxidation.
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| http://dx.doi.org/10.1039/d0ra05287f | DOI Listing |
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