Stability and reactivity improved bimetallic 2D metal organic frameworks for electrocatalytic degradation of p-acetaminophenol

Abstract

The blooming consumption and disposal of p-acetaminophenol (APAP) calls for green technology for pollution control with high efficiency. In this study, series eco-friendly bimetallic 2D Metal-Organic Frameworks (MOFs)—(NixCuy)HITP were prepared as anode materials for APAP electrocatalytic degradation. With the co-existence of bimetallic centers, about 11–18 % enhanced performance was obtained by comparing with Ni3(HITP)2 and Cu3(HITP)2, resulting in 98 % APAP removal in 40 min. For mechanism, both experiment (Ni/Cu modulation and H2SO4 etching) and density functional theory (DFT) results proved the contributions of metal sites for electron transfer acceleration, rather than as direct active sites. The accelerated electron transfer then bloomed the secondary active species generation, including active chlorine, •O2− and 1O2. Meanwhile, the superior stability and reactivity of (NixCuy)HITP encountered attractive pH tolerance and recycle possibility for practical application. The detailed APAP degradation pathways were further provided according to GC-MS results to complete whole process mechanism discussion from “reaction site” to “activated species ’’ to “ pollutant degradation pathways”.