Optimizing the CeO2-MnO2 interface via H2O2 etching for surface lattice oxygen activation in the plasma catalytic degradation of trimethylamine

Abstract

Trimethylamine (TMA) is a nitrogen-containing malodorous gas that is toxic and hazardous to humans. Plasma catalysis is a promising technique for removing low-concentration malodorous gases. CeO2/MnO2 nanowires with different Ce–Mn contact interfaces prepared by impregnation, physical mixing, and H2O2 etching were investigated for TMA degradation in a plasma catalytic system. The CMO-H sample prepared by H2O2 etching achieved a removal efficiency of 100% at 98 J/L, demonstrating the highest activity. Characterization revealed that H2O2 etching led to the uniform formation of CeO2 nanoparticles on MnO2, promoting the transfer of electrons between Ce and Mn species. Surface lattice oxygen and high-valent manganese were confirmed to be the main active species, consistent with the Mars van Krevelen mechanism. Density functional theory calculations confirmed that the CMO-H sample exhibited the lowest oxygen vacancy formation energy. In situ plasma diffuse reflection infrared transform spectroscopy analysis and gas chromatography-mass spectrometry results showed the possible degradation pathway of TMA. In summary, the H2O2 etching process optimized CeO2-MnO2 interactions and improved the utilization of lattice oxygen active sites, enhancing the catalytic degradation of TMA and providing new insights into the design of an efficient plasma catalytic system for environmental remediation.