Herein, we for the first time demonstrate the synthesis of exfoliated C₄N nanosheets via a top–down approach and exploit their use as a new class of organic polymeric catalyst for the oxygen reduction reaction (ORR). The obtained C₄N nanosheets are semi–conductive with a small band gap of 1.41 eV and contain abundant pyrazine–nitrogen moieties uniformly distributed throughout C₄N. Density function theory calculations reveal that the intramolecular charge transfer induced by pyrazine–nitrogen in C₄N enables effective charge redistribution to activate the conjugated structure and facilitate the oxygen adsorption, while the exfoliated sheet–like C₄N formation renders improved electrochemical active surface area and results in high exposure of active sites. As a result, despite the bulk C₄N is not active, the sheet–like C₄N yield markedly improved ORR performance, even on a par with the commercial Pt/C catalyst. Our recent findings not only enrich the family members of two–dimensional conjugated polymer nanosheets but also open up new opportunity to explore new metal–free organic polymeric materials for efficient oxygen reduction catalysis and beyond.

在此，我们首次证明剥离C的合成₄经由前N个纳米片-向下的方法和利用其作为一类新的氧还原反应（ORR）有机聚合催化剂的使用。所述获得的C ₄ Ñ纳米片是半-导通1.41电子伏特的带隙小，并含有丰富吡嗪-整个Ç均匀分布的氮部分₄ N.密度函数理论计算表明诱导吡嗪的分子内电荷转移-在C在氮气₄Ñ使有效电荷再分配来激活共轭结构和促进氧吸附，而剥离的片材-例如C ₄ ñ形成使得改进的电化学活性表面积和在高曝光活性位点的结果。结果，尽管大部分的C ₄ N都没有活性，该薄板（像C ₄ N一样）仍显着提高了ORR性能，即使与商用Pt / C催化剂相比也是如此。我们最近发现不仅丰富了两个家庭成员-二维共轭聚合物纳米片还要开辟新的机会，探索新金属-高效的氧还原催化和超过自由有机聚合材料。