Ball-milled layer double hydroxide as persulfate activator for efficient degradation of organic: Alkaline sites-triggered non-radical mechanism

Abstract

Considerable efforts have been put into enhancing the activation performance of peroxydisulfate (PDS) by catalysts toward oxidative degradation of organic pollutants, while the oxidative selectivity is somehow overlooked. Here, we reported an enhanced non-radical oxidation pathway of PDS, activated by ball-milled Mg/Al-layered double hydroxide (BM-LDH), to reconcile the selectivity and reactivity. EPR and quenching experiments suggested that 1O2 dominated the oxidative pathway for phenol degradation without generating carcinogenic halide by-products. Multiple interfacial characterizations and density functional theory (DFT) calculations revealed that BM-LDH played dual roles in PDS activation: (1) the interlaminar BM-LDH allowed PDS intercalation to form complexed PDS, resulting in decreases in the activation barrier of PDS; (2) abundant terminal hydroxyls in the layers of BM-LDH acted as alkaline-activation sites that can efficiently activate PDS to generate 1O2 toward phenol degradation. Ball-milling treatment of LDH refined the structural hierarchy of LDH to create pore volumes, which greatly enhanced the diffusion of phenol to the intercalated PDS, resulting in more than twice the reaction rate for phenol degradation. This study provided a promising approach to simultaneously control over the reactivity and selectivity toward PDS activation that are critical for the degradation of organic pollutants particularly in drinking water treatment.