▎ 摘　　要

Innovations in energy storage and conversion technologies are closely dependent on developing superior materials that can be used in this field. Here, we present an indus-trially scalable and low-cost solvothermal method for synthesizing Si-N-co-doped (Si-N-GN) and N-doped graphene (N-GN) with a high specific surface area of 523 m2 g-1 and 1289 m2 g-1, respectively. Silicon atoms were successfully incorporated into the 2D gra-phene at a doping rate of 2.28 at.% via Si-C, Si-N, and Si-O bonds, thanks to the decar-bonylation of N,N-dimethyl formamide (DMF) into dimethylamine and highly reactive carbonyl at the solvothermal conditions. The Si-N-GN exhibited an average electron transfer number of 3.83 e- per mole of O2 in a wide potential range with similar on-set potential (0.988 V vs. 1.012 V), greater methanol tolerance capability, and higher diffu-sion limiting current density (7.2 vs. 6.5 mA cm-2 at 0.4 V) for oxygen reduction reaction (ORR) in alkaline electrolytes compared to the commercial Pt/C catalyst. The improved ORR performance of Si-N-GN was attributed to the effectively decreased adsorption energy of O2 on SiC4 and SiN1C3 type bondings supported by the density functional theory (DFT) cal-culations based on the model created according to the XPS results. The promising electrocatalytic activity of Si-N-GN for ORR could also be enlarged to other electrochemical applications, including metal-air batteries.(c) 2023 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.