H₂O₂ activation by two-dimensional metal-organic frameworks with different metal nodes for micropollutants degradation: Metal dependence of boosting reactive oxygen species generation

The existence of organic micropollutants (OPMs) in water poses a considerable threat to the environment. A centralized approach towards pollutants abatement has dominated over the recent decades wherein heterogeneous Fenton-like based advanced oxidation processes can be a promising technology. The application of engineered nanomaterials offers more opportunities to enhance their catalyst properties. This study synthesizes a series of ultrathin two-dimensional (2D) Metal-organic frameworks (MOFs) nanosheets with tunable metal clusters. The formation of reactive oxygen species (^•OH and ¹O₂) can be significantly boosted via transferring the adsorbed H₂O₂ onto the solid-liquid interface by systematically tuning the metal species. The Co-MOF nanosheets exhibited an ultrafast degradation kinetic for BPA with a rate of 2.23 min⁻¹ (4.98 times higher than that of the bulk MOF) and TOF (turnover frequency) value of 9.99 min⁻¹, which are observably greater than that of the existing materials reported to date. Density functional theory simulation and experimental results unravel the mechanism for ROS formation, which is strongly metal-depend. We further loaded the powder onto a flow-through poly (vinylidene fluoride) (PVDF) microfiltration membrane and observed that the representative OPMs could be rapidly degraded, indicating promising properties for practical application.