Developing efficient electrocatalysts for energy storage and oxygen reduction reaction (ORR) is of great significance for the utilization of renewable energy. In particular, designing catalysts with both promising activity and long stability for ORR in pH-universal electrolytes still remain as a tremendous challenge. To tackle such a problem, metal-free nitrogen and sulfur co-doped porous carbon sheet (NSPCS) was rationally designed in this work in order to integrate the two reported routes of enhancing the electrocatalytic activity of graphene. The as-prepared NSPCS has an onset potential of 0.89 V vs. RHE, and half-wave potential E_1/2 ≈ 0.75 V during ORR in acidic solution, making it as the most active ORR catalyst. Moreover, the resulting NSPCS also shows a 0.03 V positive shift of half-wave potential than commercial Pt/C for ORR and excellent charge capacitive performance in alkaline media. Electron microscopy revealed high degree of defects on NSPCS surface. This, coupled with synergistic doping effects of nitrogen and sulfur, optimized the active sites and charge transfer, rationalized the outstanding performance in both oxygen reduction reactions and supercapacitors.

开发用于储能和氧还原反应（ORR）的高效电催化剂对可再生能源的利用具有重要意义。尤其是，在通用pH的电解质中，设计具有理想的活性和ORR长期稳定性的催化剂仍然是一个巨大的挑战。为了解决这个问题，在这项工作中合理设计了无金属氮和硫共掺杂多孔碳片（NSPCS），以整合两种报道的增强石墨烯电催化活性的途径。所制备的NSPCS的起始电势为RHE 0.89 V，半波电势E _1/2在酸性溶液中进行ORR时≈0.75 V，使其成为活性最高的ORR催化剂。此外，对于ORR，所得的NSPCS还显示出比商用Pt / C高0.03 V的半波电势正向偏移，并且在碱性介质中具有出色的充电电容性能。电镜观察发现NSPCS表面存在高度缺陷。这与氮和硫的协同掺杂作用相结合，优化了活性位点和电荷转移，使氧还原反应和超级电容器的出色性能合理化。