New insights into enhanced electrochemical advanced oxidation mechanism of B-doped graphene aerogel: Experiments, molecular dynamics simulations and DFT

B-doped graphene, as an efficient and environmental-friendly metal-free catalyst, has aroused much attention in the electrochemical advanced oxidation process (EAOP), but the bottleneck in this field is to determine the relationship between the surface structure regulation and activity of catalysts. Herein, the B-doped graphene aerogel (BGA) fabricated gas diffusion electrode was prepared and used as a cathode for EAOP to remove tetracycline (TC). Higher free radical yield (169.59 mu M), faster reaction speed (0.35 min-1) and higher TC removal rate (99.93%) were found in the BGA system. Molecular dynamics simulation unveiled the interaction energy of BGA was greater than the raw graphene aerogel (GA). The adsorption-activation process of H2O2 and the degradation process of TC occurred in the first adsorption layer of catalysts. And both processes turned more orderly after B doping, which accelerated the reaction efficiency. Results of density functional theory displayed the contribution of three B-doped structures to improve the binding strength between H2O2 and BGA was: -BCO2 (-0.23 eV) > -BC2O (-0.16 eV) > -BC3 (-0.09 eV).-BCO2 was inferred to be the main functional region of H2O2 in-situ activation to hydroxyl radical (center dot OH), while-BC2O and-BC3 were responsible for improving H2O2 production.