Synergy of oxygen reduction for H 2 O 2 production and electro-fenton induced by atomic hydrogen over a bifunctional cathode towards water purification.

In the Electro-Fenton (EF) process, hydrogen peroxide (H 2 O 2 ) is produced in situ by a two-electron oxygen reduction reaction (2e ORR), which is further activated by electrocatalysts to generate reactive oxygen specieces (ROS). However, the selectivity of 2e transfer from catalysts to O 2 is still unsatisfactory, resulting in the insufficient H 2 O 2 availability. Carbon based materials with abundant oxygen-containing functional groups have been used as excellent 2e ORR electrocatalysts, and atomic hydrogen (H*) can quickly transfer one electron to H 2 O 2 in a wide pH range and avoiding the restrict of traditional Fenton reaction. Herein, nickel nanoparticles growth on oxidized carbon deposited on modified carbon felt (Ni/C o @CF AO ) was prepared as a bifunctional catalytic electrode coupling 2e ORR to form H 2 O 2 with H* reducing H 2 O 2 to produce ROS for highly efficient degradation of antibiotics. Electrochemical oxidation and thermal treatment were used to modulate the structure of carbon substrates for increasing the electro-generation of H 2 O 2 , while H* was produced over Ni sites through H 2 O/H + reduction constructing an in-situ EF system. The experimental results indicated that 2e ORR and H* induced EF processes could promote each other mutually. The optimized Ni/C o @CF AO with a Ni:C mass ratio of 1:9 exhibited a high 2e selectivity and H 2 O 2 yield of 49 mg L -1 . As a result, the designed Ni/C o @CF AO exhibited excellent electrocatalytic ability to degrade tetracycline (TC) under different aqueous environmental conditions, and achieved 98.5% TC removal efficiency within 60 min H 2 O 2 and H* were generated simultaneously at the bifunctional cathode and react to form strong oxidizing free radicals •OH. At the same time, O 2 gained an electron to form •O 2 - , which could react with •OH and H 2 O to form 1 O 2 , which had relatively long life (10 -6 ∼10 -3  s), further promoting the efficient removal of antibiotics in water.