Nanocarbon materials recognized as effective and inexpensive catalysts for independent electrochemical reactions, are anticipated to possess a broader spectrum of multifunctionality toward oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). A rational design of trifunctional nanocarbon catalyst requires balancing the heteroatoms-doping and defect-engineering to afford desired active centers and satisfied electric conductivity, which however is conceptually challenging while desires in-depth research both experimentally and theoretically. This work reports a N,B-codoped graphitic carbon nanocage (NB-CN) with graphitic yet defect-rich characteristic as a promising trifunctional electrocatalyst through a facile thermal pyrolysis assisted in-situ catalytic graphitization (TPCG) process. Density functional theory (DFT) calculations are conducted, for the first time, to demonstrate that the best performance for ORR/OER and HER can be originated from the configuration with B meta to a pyridinic-N, which presents a minimum theoretical overpotential of 0.34 V for ORR, 0.39 V for OER, and a lowest Gibbs free-energy (ΔG_ads) of 0.013 eV for HER. A primary zinc-air battery is assembled presenting a maximum power density of 320 mW cm⁻² along with excellent operation durability, evidencing great potential in practical applications.

被认为是用于独立电化学反应的有效且廉价的催化剂的纳米碳材料预期具有针对氧还原反应（ORR），氧释放反应（OER）和氢释放反应（HER）的更广泛的多功能性。合理设计三官能纳米碳催化剂需要平衡杂原子掺杂和缺陷工程，以提供所需的活性中心和令人满意的电导率，然而，这在概念上具有挑战性，同时需要在实验和理论上进行深入研究。这项工作报告了一种N，B掺杂的石墨碳纳米笼（NB-CN），其具有石墨但富含缺陷的特性，是一种通过简便的热热解辅助原位催化石墨化（TPCG）工艺成为有前途的三功能电催化剂。元到吡啶-N，其呈现出最小理论过电位0.34V的用于ORR，0.39 V代表OER，和最低吉布斯自由能的（ΔG_广告0.013电子伏为HER的）。组装的一次锌-空气电池具有320 mW cm ^-2的最大功率密度以及出色的操作耐久性，在实际应用中显示出巨大的潜力。