Developing durable and efficient doped-type carbon electrocatalysts with diverse heteroatoms or transition metals for oxygen reduction reaction (ORR) has captured increasing attention for their incredible electrocatalytic properties. However, compared to multiple-atom-doped carbon matrix, the introduction of single-type atoms into carbon skeletons provides little benefit to enhancing ORR activity. On the basis of this consideration, we successfully fabricated a cobalt (Co) and nitrogen (N) dual-doped porous carbon (Co@C-N) hybrid with multiple active sites by a facile strategy of combined hydrothermal reaction with thermolysis. As a comparison, porous nitrogen-doped carbon (C@N) was obtained by a similar method. Electrochemical tests confirm that the Co@C-N-120-900 exhibits the best ORR performance in alkaline media with the positive onset potential (E_onset) of 0.956 V vs. RHE (only 12 mV more negative than Pt/C), the high half-wave potential (E_1/2) of 0.851 V vs. RHE (24 mV more positive than 20 wt% Pt/C), superior selectivity (a four-electron-dominant process), and smaller Tafel slope (57 mV dec⁻¹). Meanwhile, as-synthesized Co@C-N-120-900 catalyst shows greater durability and significantly greater methanol tolerance than Pt/C catalyst. Our experiments indicate that the better overall ORR performance for Co@C-N-120-900 could be caused by the synergistic effect of multiple active components (single Co atom, Co–N_x and plentiful pyridinic-N), high BET specific surface area (1080 m² g⁻¹) and porous structures. Thus, the Co@C-N-120-900 catalyst is expected to be a cost-efficient and promising electrocatalyst in the field of the sustainable energy application, and this work might provide some directions for fabricating advanced energy storage materials.

中文翻译：

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多种活性成分，协同驱动的钴和氮钴掺杂的多孔碳作为高性能的氧还原电催化剂

开发具有多种杂原子或过渡金属以进行氧还原反应（ORR）的耐用高效的掺杂型碳电催化剂，因其令人难以置信的电催化性能而受到越来越多的关注。然而，与多原子掺杂的碳基质相比，将单型原子引入碳骨架对提高ORR活性几乎没有好处。基于这种考虑，我们通过水热反应与热解相结合的简便策略成功地制备了具有多个活性位的钴（Co）和氮（N）双掺杂多孔碳（Co @ CN）杂化体。作为比较，通过类似的方法获得了多孔的氮掺杂碳（C @ N）。È_发病0.956的V）与RHE（只有12毫伏比的Pt / C更负），高半波电势（Ë _1/2 0.851的V）与RHE（24毫伏超过20重量％Pt /正C），优异的选择性（四电子主导过程）和较小的塔菲尔斜率（57mV dec ^-1）。同时，合成后的Co @ CN-120-900催化剂比Pt / C催化剂具有更好的耐久性和更强的甲醇耐受性。我们的实验表明，Co @ CN-120-900的总体ORR性能更好是由多种活性成分（单个Co原子，Co-N _x和大量吡啶基-N），高BET比表面积（ 1080 m ²克^-1）和多孔结构。因此，在可持续能源应用领域中，Co @ CN-120-900催化剂有望成为一种经济高效的有前途的电催化剂，这项工作可能为制造先进的储能材料提供一些指导。