Abstract
The strong metal-support interaction (MSI) has been widely attributed to enhanced catalytic activity. However, this attribution might be wrong in catalytic ozonation, since MSI that is too strong might impede the activation of electron-poor ozone molecules. Herein, we reported a strategy to subtly modulate the Mn-O-Si interaction by intercalating the carbon film between the silica support and active manganese oxide. When using MnO(x)/0.5C/SiO(2) with the moderate MSI as a catalyst in the catalytic ozonation of refractory paracetamol (PCM), 91.1 ± 2.4% of PCM was removed within 30 min, about 30% higher than that using the catalyst of MnO(x)/SiO(2) with a strong MSI. Moreover, the reaction rate reached 8.01 × 10(-2) min(-1), 2.2 and 1.3 times that with MnO(x)/SiO(2) and MnO(x)/1C/SiO(2), respectively. Importantly, further integration of MnO(x)/0.5C/SiO(2) into membrane filtration achieved high rejections of PCM (>94.3%) under various realistic water scenarios during a continuous 12 h operation, demonstrating strong resistance to environmental matrices interference. Experimental and theoretical evidence revealed that the moderate MSI resulted in the high dispersion of active MnO(x) nanoclusters in the size of 2.3-4.4 nm and promoted the adsorption of ozone over MnO(x) and its dissociation into surface *O, (•)OH, (•)O(2)(-), and (1)O(2) for decontamination. As a constructive work, this study revealed the significance of MSI in catalytic ozonation and offered a simple regulation method for constructing active interfaces of metal-supported catalysts.