Metal‐Free Multi‐Heteroatom‐Doped Carbon Bifunctional Electrocatalysts Derived from a Covalent Triazine Polymer,Small

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Metal‐Free Multi‐Heteroatom‐Doped Carbon Bifunctional Electrocatalysts Derived from a Covalent Triazine Polymer
Small ( IF 13.0 ) Pub Date : 2020-11-03 , DOI: 10.1002/smll.202004342
Yong Zheng ₁ , Hui Song ₁ , Shan Chen ₁ , Xiaohui Yu ₁ , Jixin Zhu ₂ , Jingsan Xu ₃ , Kai A. I. Zhang ₄ , Chao Zhang ₁ , Tianxi Liu _{1,

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Affiliation

The construction of multi‐heteroatom‐doped metal‐free carbon with a reversibly oxygen‐involving electrocatalytic performance is highly desirable for rechargeable metal‐air batteries. However, the conventional approach for doping heteroatoms into the carbon matrix remains a huge challenge owing to multistep postdoping procedures. Here, a self‐templated carbonization strategy to prepare a nitrogen, phosphorus, and fluorine tri‐doped carbon nanosphere (NPF‐CNS) is developed, during which a heteroatom‐enriched covalent triazine polymer serves as a “self‐doping” precursor with C, N, P, and F elements simultaneously, avoiding the tedious and inefficient postdoping procedures. Introducing F enhances the electronic structure and surface wettability of the as‐obtained catalyst, beneficial to improve the electrocatalytic performance. The optimized NPF‐CNS catalyst exhibits a superb electrocatalytic oxygen reduction reaction (ORR) activity, long‐term durability in pH‐universal conditions as well as outstanding oxygen evolution reaction (OER) performance in an alkaline electrolyte. These superior ORR/OER bifunctional electrocatalytic activities are attributed to the predesigned heteroatom catalytic active sites and high specific surface areas of NPF‐CNS. As a demonstration, a zinc‐air battery using the NPF‐CNS cathode displays a high peak power density of 144 mW cm⁻² and great stability during 385 discharging/charging cycles, surpassing that of the commercial Pt/C catalyst.

中文翻译：

共价三嗪聚合物衍生的无金属多杂原子掺杂碳双功能电催化剂

具有可逆地涉及氧气的电催化性能的多杂原子掺杂的无金属碳的构造对于可再充电金属空气电池是非常理想的。然而，由于多步后掺杂程序，将杂原子掺杂到碳基质中的常规方法仍然是巨大的挑战。在这里，开发了一种自模板碳化战略，以制备氮，磷和氟三掺杂碳纳米球（NPF-CNS），在此过程中，富含杂原子的共价三嗪聚合物用作含C的“自掺杂”前体。，N，P和F元素同时使用，避免了繁琐且效率低下的后掺杂程序。引入F可以增强所得催化剂的电子结构和表面润湿性，有利于改善电催化性能。经过优化的NPF-CNS催化剂具有出色的电催化氧还原反应（ORR）活性，在通用pH值条件下的长期耐久性以及在碱性电解质中出色的氧释放反应（OER）性能。这些卓越的ORR / OER双功能电催化活性归因于NPF-CNS的预先设计的杂原子催化活性位点和高比表面积。作为演示，使用NPF-CNS阴极的锌空气电池显示出144 mW cm的高峰值功率密度这些卓越的ORR / OER双功能电催化活性归因于NPF-CNS的预先设计的杂原子催化活性位点和高比表面积。作为演示，使用NPF-CNS阴极的锌空气电池显示出144 mW cm的高峰值功率密度这些卓越的ORR / OER双功能电催化活性归因于NPF-CNS的预先设计的杂原子催化活性位点和高比表面积。作为演示，使用NPF-CNS阴极的锌空气电池显示出144 mW cm的高峰值功率密度在385个放电/充电循环中具有^−2的高稳定性，超过了商用Pt / C催化剂的稳定性。

更新日期：2020-11-27

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