Novel MOF-derived Fe/CoNHDC-400@GF cathode with improved in-situ catalytic degradation of chloroquine phosphate during heterogeneous electro-Fenton process

Abstract

The preparation of stable and high-efficiency heterogeneous electro-Fenton cathodes for the treatment of pollutants is important for environmental remediation. Herein, a novel N-doped MOF-derived Fe/Co bimetallic catalyst was in-situ grown on graphite felt (GF) surface to yield a composite cathode Fe/CoNHDC-400@GF for use in electro-Fenton process. The introduction of cobalt accelerated electron transfer due to existing polyvalent metals. The synergistic effect between Co0, CoⅡ, CoШ, FeⅡ, and FeШ enabled the continuous generation of reactive oxygen species (•OH and •O2−). Under near-neutral conditions (pH=6.5), complete removal of 10 mg L−1 chloroquine phosphate (CQP) was achieved within 60 min. Additionally, efficient removal was also achievable over a wide pH range (pH=3–11). The mechanistic investigations indicated •OH as a major active oxygen species for CQP degradation. A combination of the experimental results with density functional theory calculations (DFT) clarified the degradation pathway and intermediate products of CQP. Moreover, the toxicity of degradation products significantly reduced. Overall, valuable insights on preparing composite cathodes grown in-situ for efficient removal of refractory pollutants from wastewater during the heterogeneous electro-Fenton process were provided, useful for future consideration.