Mechanistic insights into efficient peroxymonosulfate activation by NiCo layered double hydroxides

Abstract

The efficient removal of organic refractory pollutants such as dyes and antibiotics in wastewater is crucial for protecting the environment and human health. In this work, a NiCo-layered double hydroxide (NiCo-LDH) with a uniform microspherical, hierarchical structure and a high surface area was successfully synthesized as an effective peroxymonosulfate (PMS) activator for the degradation of various organic dyes and antibiotics. The influence of various parameters on the catalytic activity of the NiCo-LDH was determined. Radical scavenger studies unveiled the major reactive oxygen species (ROSs) generated in the NiCo-LDH/PSM system to be ¹O₂, SO₄^•-, and O₂^•-. Ex-situ X-ray photoelectron spectroscopy (XPS) analysis uncovered the role of Co sites and oxygen vacancy as active sites and revealed the reversible redox properties of NiCo-LDH based on Co²⁺/Co³⁺ cycles. The activation mechanism and Rhodamine B (RhB) degradation pathways were experimentally studied and proposed. The NiCo-LDH is highly versatile, reusable and stable as shown by post-catalysis characterizations. This work shows the excellent catalysis performances and provides insights into the activation mechanism of PMS by NiCo-LDH for organic pollutant remediation.

Keywords: Ni–Co layered Double hydroxide; Organic dyes; Peroxymonosulfate activation; Rhodamine B; Singlet oxygen; olvothermal synthesis.