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首页> 外文期刊>RSC Advances >Nitrogen doped nanoporous graphene: an efficient metal-free electrocatalyst for the oxygen reduction reaction
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Nitrogen doped nanoporous graphene: an efficient metal-free electrocatalyst for the oxygen reduction reaction

机译：氮掺杂纳米多孔石墨烯：一种有效的无金属电催化剂，用于氧还原反应

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摘要

The oxygen reduction reaction (ORR) is an important half reaction, which occurs at the cathode within a fuel cell and limits their range of applications due to slow electrochemical kinetics. To overcome this issue, electrocatalysts are sought, which need to be an alternative to expensive and unsustainable metallic catalysts. Herein we report the synthesis of nitrogen doped nanoporous graphene (NPG), which is a competitive alternative to currently employed metallic catalysts. The NPG is synthesised through a chemical vapour deposition methodology followed by a chemical functionalization step introducing oxygen functional groups (carbonyl and hydroxyl groups), which is then doped with nitrogen via orthophenylenediamine (OPDA). The NPG is physiochemically and electrochemically characterised. The NPG demonstrates outstanding electrocatalytic activity towards the ORR in alkaline media proceeding via a favourable 4-electron pathway and is comparable to commercially available platinum-carbon (20%). We demonstrate that the electrochemical activity of the NPG is tailorable such that through increased nitrogen doping the ORR transforms from a 2-electron process to that of the favourable 4-electron process via increasing the proportion of pyridinic nitrogen while the content of graphitic nitrogen remains almost constant. The NPG exhibits excellent electrochemical performance towards the ORR in alkaline media, long-term stability and appropriate methanol crossover as benchmarked to commercialised Pt/C electrodes; this outstanding electrocatalytic activity is related to the high proportion of defects, high porosity and (pyridinic) doping.
机译：氧还原反应（ORR）是一个重要的半反应，其在燃料电池内的阴极发生并限制其由于电化学动力学慢的应用范围。为了克服这个问题，寻求电催化剂，需要是昂贵和不可持续的金属催化剂的替代品。在此，我们报告了氮掺杂纳米多孔石墨烯（NPG）的合成，其是目前使用的金属催化剂的竞争替代品。通过化学气相沉积方法合成NPG，然后通过化学官能化步骤引入氧官能团（羰基和羟基），然后通过正苯基二胺（OPDA）掺杂氮气。 NPG是理化和电化学表征的。 NPG通过良好的4型电子通路表明朝向碱性介质中的ORR中出色的电催化活性，并且与市售的铂 - 碳（20％）相当。我们证明NPG的电化学活性可批定，使得通过增加氮气从2孔的氮气转化为有利的4 - 电子过程的变换，通过增加吡啶氮的比例，而石墨氮的含量几乎仍然存在持续的。 NPG对碱性介质的ORR具有优异的电化学性能，长期稳定性和适当的甲醇交叉，与商业化PT / C电极的基准测试;这种出色的电催化活性与高比例的缺陷，高孔隙度和（吡啶碱）掺杂有关。

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