Surface Lattice Oxygen Activation by Nitrogen-Doped Manganese Dioxide as an Effective and Longevous Catalyst for...

Oxygen vacancy plays an important role in catalytic oxidation of formaldehyde (HCHO), but the inherent drawback of its thermodynamic instability causes the deactivation of catalysts. Hence, improving the thermodynamic stability of oxygen vacancy is a crux during HCHO oxidation. Here, a novel and simple nitrogen doping of MnO₂/C catalyst is designed for HCHO oxidation at room temperature. The surface lattice oxygen of MnO₂ will be activated by nitrogen-doping, which acts as active sites for HCHO oxidation and solves the thermodynamic instability issue of oxygen vacancy. Furthermore, carbon is doped with nitrogen to promote electron transfer and accelerate the HCHO oxidation process. Therefore, the catalytic activity and stability of the catalyst can be significantly promoted, which can completely remove ∼1 ppm HCHO in the tank within 3 h, and remains highly active after 5 cycles at room temperature (RH = 55%). In addition, the excellent removal performance over the prepared catalyst is also attributed to abundant surface oxygen species, amorphous crystallinity, and low reduction temperature. In situ diffuse reflectance infrared Fourier transform spectrometry (DRIFTS) and density functional theory (DFT) calculations reveal the reaction mechanism of HCHO. This strategy provides crucial enlightenment for designing novel Mn-based catalysts for application in the HCHO oxidation field.