Waste biomass-derived N, P co-doping carbon aerogel-coated CoxFe1−xP with modulated electron density for efficient electrooxidation of contaminants.

The Fe-modulated Co x Fe 1−x P@NPC exhibits excellent electrooxidation performance. [Display omitted] • The N content of NPC is increased via WLSH as precursor to increase its catalytic site density. • Co x Fe 1−x P@NPC exhibits excellent electrooxidation performance for TCH removal. • Radical generation capacity of Co x Fe 1−x P@NPC can be modulated with Fe modulation. • The mechanism for electrooxidation activity of Co x Fe 1−x P@NPC is reasonably revealed. Developing low-cost, green, high-performing electrode materials to address environmental pollutants and the energy crisis is significant but challenging. Herein, the bimetallic iron cobalt phosphide coated in waste biomass-derived N, P co-doping carbon (Co x Fe 1−x P@NPC) is constructed. Furthermore, the active site density and the water decomposition energy barrier of surface-coated NPC are modulated by optimizing the electronic structure of Co x Fe 1−x P via doping engineering. The Fe-modulated Co x Fe 1−x P@NPC exhibits a hierarchical porous self-supporting structure and excellent physical & chemical properties with excellent electrooxidation performance, achieving over 95% removal of TCH within 60 min. The density functional theory (DFT) calculations further confirms that N carries more positive charge and P carries more negative charge in the NPC of Co x Fe 1−x P@NPC with Fe modulation, which can promote the adsorption and dissociation of water molecules. Of note, Co 0.75 Fe 025 P@NPC displays a low water dissociation energy barrier to produce ·OH and a high energy barrier to produce O 2 than its counterparts. This study offers new insight into controllable modulation of biomass carbon-based composite electrode catalytic activity for high-efficiency degradation of contaminants. [ABSTRACT FROM AUTHOR]