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Reaction mechanism of N-(4-hydroxyphenyl)ethanamide electrodegradation via phosphorus-graphene prepared from triphenylphosphine: Generation and destruction of the reactive species
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•P could increase the transportation rate of charge and specific surface area.•P-GN as catalyst could accelerate the generation of active chlorine for oxidation.•The most active P was -CPO3, P-C, P-O, and -PO2 species.•DFT and experiment results confirmed the destruction of active chlorine by O2.
Electrocatalysis as effective method for organic pollutants treatment, is greatly depended on the anode material. Graphene as wide used inorganic metal-free material could greatly improve by heteroatom doping. In this study, phosphorus-doped graphene (P-GN) was successfully prepared with triphenylphosphine as the phosphorus source and applied in the electrocatalytic oxidation of N-(4-hydroxyphenyl)ethanamide. The doping morphology of phosphorus was controlled by annealing temperature, and rising temperature could gradually alter the morphology of phosphorus from P-C to P-O. P-GN (20%–500 °C) had the best catalytic efficiency (91%) after 90 min of reaction, and the most active P species were confirmed as -CPO3, P-C, P-O, and -PO2 (from XPS). Those P species as catalyst could accelerate the generation of active chlorine for oxidation. However, the existence of O2 will weaken the seizing of electrons and increase the energy barrier of Cl- connection. The discussion of “P species regulate → P active species → active chlorine generation and destruction” could provide deep understanding of underlying mechanism.