RESUMEN

In the context of the air quality co-benefits of carbon neutrality, conventional strategies for the end-of-pipe control reduction of volatile organic compounds (VOCs) towards carbon dioxide (CO2) need to be revised more realistically. This study explored the synergetic removal of carbonyls with low carbon emission by amine-functionalized manganese dioxide (MnO2), obtained with a method involving freezing-thawing cycles. Molecular-level characterization revealed that an ordered array of interfacial water dimers (H5O2+, a class of water-proton clusters) on the MnO2 surface enhanced the robust bonding of metal sites with amino groups. Amine-functionalized MnO2 can be negatively charged under environmental acidity to further interfacial proton-coupled electron transfers. Cooperativity in the interfacial chemical processes facilitated the selective conversion of carbonyl carbons to bicarbonated amides (NH3+HCO3-) as a reservoir of CO2. Compared with a commercially used 2,4-dinitrophenylhydrazine (DNPH) control, the nearly complete removal of a priority carbonyl mixture containing formaldehyde, acetaldehyde, and acetone was attained synergically. The secondary organic compounds in the gas phase and CO2 off-gas were suppressed.