New carbon morphologies are desirable in the development of high-performance carbon-based electrocatalysts for cathodic oxygen reduction reaction (ORR) of polymer electrolyte membrane fuel cells. In this work, a carbon semi-tube (CST) is successfully constructed by polymerizing m-phenylenediamine (mPDA) using surfactant-assembled micelles as a soft template. After pyrolysis, the CST morphology is retained in the formed N-doped CST (N-CST) catalyst. This mPDA-induced catalyst can provide rich micropores, high N-content, and good conductivity, imbuing it with superior catalytic ORR activity, stability, and methanol tolerance to the commercial Pt/C catalyst. By using such a metal-free N-CST as a cathode catalyst, an alkaline polymer electrolyte fuel cell exhibits a maximum power density of about 200 mW cm⁻². Furthermore, density functional theory (DFT) calculations suggest that high curvature can be greatly conducive to the excellent catalytic ORR activity by the induced strong OOH∗ adsorption on active sites through a strong dipole-electric field interaction.

在开发用于聚合物电解质膜燃料电池的阴极氧还原反应 (ORR) 的高性能碳基电催化剂时，需要新的碳形态。在这项工作中，通过使用表面活性剂组装的胶束作为软模板聚合间苯二胺 (mPDA) ，成功构建了碳半管 (CST) 。热解后，CST 形态保留在形成的 N 掺杂 CST (N-CST) 催化剂中。这种mPDA诱导的催化剂可以提供丰富的微孔、高N含量和良好的导电性，使其具有优于商业Pt/C催化剂的催化ORR活性、稳定性和甲醇耐受性。通过使用这种无金属 N-CST 作为阴极催化剂，碱性聚合物电解质燃料电池的最大功率密度约为 200 mW cm^-2。此外，密度泛函理论 (DFT) 计算表明，高曲率可以通过强偶极-电场相互作用在活性位点上诱导强 OOH* 吸附，从而极大地促进优异的催化 ORR 活性。