Ammonia-coal combustion mitigates CO2 emissions, yet nitrogen oxide emissions and char nitrogen oxidation mechanisms require further study. Our research employs density functional theory to explore coal char interactions with NO, NH3, and the impact of hydroxyls (–OH) and oxygen on reduction–oxidation processes. Findings indicate oxygen aids in forming hydroxyls on coal char, facilitating NO to NO2 conversion, lowering the activation energy for ammonia-coal oxidation to NO2. Oxygen also promotes char nitrogen oxidation to NO, reducing its activation energy. In NH3/coal/O2 systems, NH3 oxidation initiates NO formation. With the increase of the temperature, the reduction rate of NO by ammonia is always higher than the production rate of NO.
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