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首页> 美国卫生研究院文献>Scientific Reports >Ice crystals growth driving assembly of porous nitrogen-doped graphene for catalyzing oxygen reduction probed by in situ fluorescence electrochemistry
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Ice crystals growth driving assembly of porous nitrogen-doped graphene for catalyzing oxygen reduction probed by in situ fluorescence electrochemistry

机译：原位荧光电化学探测多孔氮掺杂石墨烯的冰晶生长驱动组件催化氧还原

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In recent years, doped carbonaceous materials as alternative catalysts for oxygen reduction reaction (ORR) have received considerable attention due to the low cost and high CO tolerance capability. Different theoretical studies have suggested that oxygen is reduced in a rapid sequence intermediated by diverse oxygen-containing reactive intermediates (ORI). However, due to the short lifetimes of the possible ORI, direct experimental evidence is very difficult to be obtained. Here, we report the synthesis of an ultralight and porous nitrogen-doped graphene (NG) by annealing graphite oxide (GO)-melamine scaffold shaped in ice template. The resultant NG exhibits excellent electrocatalytic activity toward 4e-reduction of oxygen with the onset potential as low as −0.05 V vs. Ag/AgCl in alkaline media. Using this material as model study, sensitive in situ fluorescence spectroelectrochemistry is applied to demonstrate the presence the reactive ORI. The global ORR pathway is unraveled as stepwise electron transfer involving hydroxyl radical as the important intermediate via both inner- and outer-sphere process. This result would likely provide a new insight into the further understanding of ORR mechanism on those intrinsic carbonaceous materials.
机译：近年来，由于低成本和高CO耐受能力，掺杂碳质材料作为氧还原反应（ORR）的替代催化剂受到了广泛关注。不同的理论研究表明，氧气可以通过多种含氧反应性中间体（ORI）迅速还原。但是，由于可能的ORI的寿命短，因此很难获得直接的实验证据。在这里，我们报告通过退火在冰模板中成形的氧化石墨（GO）-三聚氰胺支架合成超轻多孔氮掺杂石墨烯（NG）。所得的NG在碱性介质中相对于Ag / AgCl表现出优异的对4e还原氧的电催化活性，其起始电位低至-0.05V。使用这种材料作为模型研究，采用灵敏的原位荧光光谱电化学来证明反应性ORI的存在。全局ORR途径是通过逐步通过内部和外部球体过程将羟基自由基作为重要中间体的电子转移而解开的。该结果可能会为进一步了解那些固有碳质材料上的ORR机理提供新的见解。

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