Research efforts on permanganate(Mn(VII))combined with redox-mediator(RM),have received increasing attention due to their significant performance for bisphenol-A(BPA)removal.However,the mechanisms underpinning BPA deg...Research efforts on permanganate(Mn(VII))combined with redox-mediator(RM),have received increasing attention due to their significant performance for bisphenol-A(BPA)removal.However,the mechanisms underpinning BPA degradation remain underexplored.Here we show the overlooked interactions between RM and BPA during permanganate oxidation by introducing an RMdN-hydroxyphthalimide(NHPI).We discovered that the concurrent generation of MnO_(2) and phthalimide-N-oxyl(PINO)radical significantly enhances BPA oxidation within the pH range of 5.0e6.0.The detection of radical cross-coupling products between PINO radicals and BPA or its derivatives corroborates the pivotal role of radical cross-coupling in BPA oxidation.Intriguingly,we observed the formation of an NHPI-BPA complex,which undergoes preferential oxidation by Mn(VII),marked by the emergence of an electronrich domain in NHPI.These findings unveil the underlying mechanisms in the Mn(VII)/RM system and bridge the knowledge gap concerning BPA transformation via complexation.This research paves the way for further exploration into optimizing complexation sites and RM dosage,significantly enhancing the system's efficiency in water treatment applications.展开更多
基金supported by the National Natural Science Foundations of China(No.22076016).
文摘Research efforts on permanganate(Mn(VII))combined with redox-mediator(RM),have received increasing attention due to their significant performance for bisphenol-A(BPA)removal.However,the mechanisms underpinning BPA degradation remain underexplored.Here we show the overlooked interactions between RM and BPA during permanganate oxidation by introducing an RMdN-hydroxyphthalimide(NHPI).We discovered that the concurrent generation of MnO_(2) and phthalimide-N-oxyl(PINO)radical significantly enhances BPA oxidation within the pH range of 5.0e6.0.The detection of radical cross-coupling products between PINO radicals and BPA or its derivatives corroborates the pivotal role of radical cross-coupling in BPA oxidation.Intriguingly,we observed the formation of an NHPI-BPA complex,which undergoes preferential oxidation by Mn(VII),marked by the emergence of an electronrich domain in NHPI.These findings unveil the underlying mechanisms in the Mn(VII)/RM system and bridge the knowledge gap concerning BPA transformation via complexation.This research paves the way for further exploration into optimizing complexation sites and RM dosage,significantly enhancing the system's efficiency in water treatment applications.
