▎ 摘　　要

The operation efficiency of electrocatalysis is strongly influenced by the characteristics of anode materials. Thus, this study on electrochemical oxidation was conducted on the basis of the oriental design of electrode materials as a means of achieving maximal and stable degradation efficiency. Heteroatom hybrid graphene oxides (GO) have recently been regarded one of the major matrices popularly used for electrode materials due to their excellent electronic properties and long-term operation stability. However, the doping species of heteroatoms are uncontrollable, and the corresponding structural effects and mechanism are unclear. Moreover, the use of electrocatalytic technology is still not a promising approach for system optimization. With the view of significantly improving operational performance, single/multiple-form S-doped GO (SGO) were designed and prepared as anodes by using radical and non-radical precursors. Bisphenol A (BPA) was used as the model contaminant to elucidate the degradation efficiency of the electrocatalytic oxidation. Results indicate that the dominated active radicals of O-2(center dot-) were more likely generated as C-SOx-C at the GO edge rather than as S in the skeleton. The source of O-2(center dot-) was not from the dissolved O-2 but from the surface functional oxygen groups and the C-SOx-C on the catalysts. However, the S in the skeleton highly contributed to the stability of the catalyst. Moreover, analytical results based on density functional theory (DFT) calculation confirmed the influence of the heteroatom species on the efficiency of the electrocatalytic oxidation and the proposed mechanism. This proposal can provide an in-depth understanding of the mechanism of electrocatalysis and an optimal operation strategy when using related carbon materials for practical applications.