N vacancies, hydrophobic sites and electron rich zone were simply regulated by doping F into g-C3N4 (CN) to accelerate photocatalytic ozonation of PFOA. Activity of F-CN was superior to that… Click to show full abstract
N vacancies, hydrophobic sites and electron rich zone were simply regulated by doping F into g-C3N4 (CN) to accelerate photocatalytic ozonation of PFOA. Activity of F-CN was superior to that of CN, with 74.3% PFOA removal by F-CN/Vis/O3 but only 57.1% by CN/Vis/O3. Experimental results and theory simulations suggested that the photogenerated hole (hvb+) oxidation with the help of N vacancies was vital for PFOA degradation. N vacancies on both CN and F-CN would trap O atom of PFOA and seize electron from α -CF2 group, which made PFOA more easily to be oxidized. Doping of F narrowed band gap, lowered the valence band position and enhanced the oxidation potential of hvb+. The hydrophobic sites would accelerate the mass transfer of O3 and PFOA, enhance O3's single electron reduction with ecb- to generate hydroxyl radicals (•OH) and reduce the recombination of hvb+-ecb-. Under the joint function of hvb+, N vacancies and •OH, PFOA degradation in F-CN/Vis/O3 proceeded through the gradually shortening of perfluoroalky chain and loss of CF2 unit. The acute and chronic toxicity of generated short-chain perfluorocarboxylic acid toward fish, green algae daphnid were predicted by ECOSAR. And the toxicity change of solutions was examined by luminescent bacteria.
               
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