Insights into carbon monoxide oxidation in supercritical H2O/CO2 mixtures using reactive molecular dynamics simulations
MJ Fan and YJ Lu, JOURNAL OF SUPERCRITICAL FLUIDS, 189, 105727 (2022).
Carbon monoxide is an important intermediate in supercritical water oxidation processes. Carbon monoxide oxidation in supercritical H2O/CO2 mixtures was investigated using reactive molecular dynamics simulations. The results show that CO mainly converts into CO2 through the reaction CO + OH & RARR; HOCO & RARR; CO2 + H. The intermediate HOCO can also react with OH or O2 to form CO2. The overall activation energies of CO oxidation in the supercritical medium range from 125.3 & PLUSMN; 4.0-159.4 & PLUSMN; 3.6 kJ/mol, which are roughly consistent with the experimental results. Supercritical water not only provides reactive free radicals for CO conversion but also acts as a third body to induce some chemical events. The high concentration of CO2 inhibits the production of OH but highlights the oxidizing action of O and HO2. Oxygen increases the amounts of OH and HO2 through the reaction H2O + O2, thereby promoting the conversion of CO.
Return to Publications page