Seeking catalysts with high density of active sites of N-doped carbon nanomaterials is desired for effective conversion of CO₂ to CO. Here, the density functional theory (DFT) calculation is employed to investigate the formation energy and chemical potential of N species from different N-containing carbon precursors. It is found that the hybrid precursors facilitate to form high density of the pyridinic-N active sites, owing to its lower formation energy of pyridinic-N. Accordingly, we develop a hybridization strategy of precursors to fabricate the N-doped porous carbon (NPC) with a pyridinic-N content of 2.86 wt% by ball milling of the poly(aniline-co-pyrrole) copolymer in the presence salt templets, followed by pyrolysis. As expected, the optimized NPC_1:0.5 exhibits an excellent activity toward CO₂RR with the CO Faradaic efficiency of ∼95.3% and a high CO current density of 4.3 mA cm⁻², higher than most of the previous reports. Besides, this NPC had CO current density of 115.9 mA cm⁻² and a long-term stability for 20 h in flow cell. The experiments and DFT calculation show that the pyridinic-N species act as active sites for CO₂RR. In addition, 2p electrons of pyridinic-N species promote *COOH intermediate release to enhance CO₂ conversion toward CO.

寻找具有高密度活性位点的 N 掺杂碳纳米材料的催化剂是将 CO ₂有效转化为 CO 所需要的。这里，密度泛函理论 (DFT) 计算被用来研究不同 N 物种的形成能和化学势。含氮碳前体。发现杂化前驱体由于其较低的吡啶-N形成能而有助于形成高密度的吡啶-N活性位点。因此，我们开发了一种前体的杂化策略，通过在盐模板存在下球磨聚（苯胺-共-吡咯）共聚物来制造吡啶-N 含量为 2.86 wt% 的 N 掺杂多孔碳（NPC），然后是热解。正如预期的那样，优化后的 NPC _{1: 0.5}表现出对 CO ₂ RR的优异活性，CO 法拉第效率约为 95.3%，CO 电流密度为 4.3 mA cm ^-2，高于之前的大多数报道。此外，该NPC的CO电流密度为115.9 mA cm ^-2并且在流通池中具有20小时的长期稳定性。实验和 DFT 计算表明，吡啶-N 物质作为 CO ₂ RR 的活性位点。此外，吡啶-N物种的2p电子促进*COOH中间释放以增强CO ₂向CO的转化。