Nitrogen-doped three-dimensional porous graphene frameworks (NGAs) are fabricated through a unique strategy of adopting the supramolecular assembly-assisted method with GO as building block, and supramolecular aggregate of self-assembled melamine and cyanuric acid as not only a “spacer” to suppress the re-stacking of graphene nanosheets but a self-sacrificial pore-forming agent as well as a nitrogen source leading to simultaneous N-doping. Supramolecular aggregates function as the structure-directing agent playing a vital role in generating the loose porous and free-stacking structure and guiding the formation of unique 3D architecture. The resulting metal-free NGA products possess high specific surface area, porous structure and free-stacking properties, and exhibit enhanced ORR performance in terms of positive half-wave potential which is only ∼43 mV lower than that of a commercial Pt/C, four-electron-transfer process, good durability and outstanding methanol poisoning tolerance. Besides, it also performs as a good support for Pt particles. Consequently, Pt/NGA catalyst displays impressive catalytic activity and stability towards efficient methanol electrooxidation reaction. This simple and robust synthetic strategy of 3D N-doped graphene has put forward a new prospect for rational synthesis of heteroatoms doped carbon materials for sustainable energy conversion applications.

氮掺杂的三维多孔石墨烯骨架（NGA）是采用独特的策略制造的，该策略采用以GO为构建基的超分子组装辅助方法，而自组装的三聚氰胺和氰尿酸的超分子聚集体不仅是“间隔物”抑制石墨烯纳米片的重新堆叠，但抑制了自牺牲成孔剂以及导致同时进行N掺杂的氮源。超分子聚集体起结构导向剂的作用，在产生松散的多孔和自由堆积的结构并指导独特的3D体系结构的形成中起着至关重要的作用。所得的不含金属的NGA产品具有较高的比表面积，多孔结构和自由堆积特性，并在正半波电位方面表现出增强的ORR性能，其仅比商用Pt / C，四电子转移工艺低约43 mV，耐用性好，并且具有出色的甲醇中毒耐受性。此外，它还可以很好地支撑Pt颗粒。因此，Pt / NGA催化剂对有效的甲醇电氧化反应显示出令人印象深刻的催化活性和稳定性。3D N掺杂石墨烯的这种简单而稳健的合成策略为合理合成杂原子掺杂的碳材料提供了新的前景，可用于可持续的能量转换应用。Pt / NGA催化剂对有效的甲醇电氧化反应显示出令人印象深刻的催化活性和稳定性。3D N掺杂石墨烯的这种简单而稳健的合成策略为合理合成杂原子掺杂的碳材料提供了新的前景，可用于可持续的能量转换应用。Pt / NGA催化剂对有效的甲醇电氧化反应显示出令人印象深刻的催化活性和稳定性。3D N掺杂石墨烯的这种简单而稳健的合成策略为合理合成杂原子掺杂的碳材料提供了新的前景，可用于可持续的能量转换应用。