The suitable structural design of carbon catalysts is a straightforward strategy to achieve a superior electrocatalytic activity for the oxygen reduction reaction. Herein, we firstly design a three‐dimensional sphere‐and‐flake‐structured Cu, N co‐doped carbon catalyst, via a template‐free method, for robust oxygen reduction reaction. The nanostructure is composed of graphene‐like nanosheets and carbon nanospheres with abundant mesopores, which can expose numerous active sites. Cu²⁺ and the copolymer of PANI and Cu²⁺ and melamine play important roles in the construction of the sphere‐and‐flake structure. By optimizing the addition of melamine, the structure of the catalyst can be successfully controlled. The as‐constructed GCNS10 material possesses a large amount of Cu‐N_x sites and exhibits an excellent electrocatalytic activity for the oxygen reduction reaction, delivering a limiting current density (6.14 mA cm⁻² at −0.1 V) and stability superior to those of commercial Pt/C materials in 0.1 M KOH solution. These satisfactory performances suggest that GCNS10 is promising as a next‐generation non‐noble‐metal oxygen reduction reaction catalyst. Besides, using an air cathode with the GCNS10 catalyst works well in a Zn‐air battery, indicating that GCNS10 can be used in such devices.

中文翻译：

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采用无模板方法设计的球形和片状结构的Cu，N共掺杂碳催化剂，用于可靠的氧还原反应

碳催化剂的适当结构设计是一种直接的策略，可以为氧还原反应实现出色的电催化活性。在此，我们首先通过无模板方法设计了一种三维球状和片状结构的Cu，N共掺杂的碳催化剂，以实现可靠的氧还原反应。纳米结构由类石墨烯纳米片和具有丰富中孔的碳纳米球组成，这些中孔可以暴露出许多活性位点。Cu ²⁺以及PANI和Cu ²⁺与三聚氰胺的共聚物在球形和片状结构的构建中起着重要作用。通过优化三聚氰胺的添加，可以成功地控制催化剂的结构。构造后的GCNS10材料具有大量的Cu-N _x在氧还原反应中具有良好的电催化活性，可提供极限电流密度（在-0.1 V时为6.14 mA cm ^-2），并具有优于市售Pt / C材料在0.1 M KOH溶液中的稳定性。这些令人满意的性能表明，GCNS10有希望成为下一代非贵金属氧还原反应催化剂。此外，将空气阴极与GCNS10催化剂一起使用在锌空气电池中效果很好，这表明GCNS10可以在此类设备中使用。