▎ 摘　　要

Layered graphene doping with abundant heteroatoms is fascinating for many applications, especially gas separation. However, it is still challenging to synthesize such material in a simple yet effective approach. In this work, we successfully synthesized a kind of layered graphene with mesoporous frameworks (20 - 100 nm) and ultrahigh N contents (32.2 - 34.1 wt%) by an in-situ templating and doping method. The key lies in the utilization of glucose as the carbon source, and melamine as the template and N source. The graphene-based mesoporous frameworks (GMFs) were then systematically investigated for SO2 capture performance. It is found that the SO2 uptakes of GMFs are considerably high, with the value of 11.14 mol/g at 298.2 K and 1.106 bar, and 4.18 mmol/ g at 298.2 K and 0.112 bar. The adsorption of SO2 on GMFs is also highly selective and reversible, based on pure and mixed gas adsorption experiments. Finally, the theoretical basis for highly efficient and selective SO2 adsorption on GMFs was established by DFT calculations and BOMD simulations.