Layered double hydroxide/carbonitride heterostructure with potent combination for highly efficient peroxymonosulfate activation

Iron-based layered double hydroxides (LDHs) have drawn tremendous attention as a promising peroxymonosulfate (PMS) activators, but they still suffer from low efficiencies limited by electrostatic agglomeration and low electronic conductivity. Herein, a MgFeAl layered double hydroxide/carbonitride (LDH/CN) heterostructure was constructed via triggering the interlayer reaction of citric acid (CA) and urea. CA as a structure-directing agent regulated the interlayer anion of MgFeAl-LDH, which enabled an interfacial tuning in the process of coupling with CN. The obtained LDH/CN heterostructure, as an efficient PMS activator, achieved nearly 100% bisphenol A (BPA) removal rate in 10 min with high specific activity (0.146 L min−1·m−2). Electron paramagnetic resonance (EPR) tests, quenching experiments, electrochemical characterization and X-ray photoelectrons spectroscopy (XPS) tests were applied to clarify the mechanism of BPA degradation. The results unraveled that the activity of the catalyst originated from the heterostructure of LDH and CN with an efficient interfacial electron transfer, which promoted the fast generation of O2•- for rapid pollutant degradation. In addition, the catalyst exhibited excellent applicability in realistic wastewater. This work offered a rational strategy for forming a heterostructure catalyst with a fine interface engineering in actual environmental cleanup.