Controlled synthesis of graphene via electrochemical route and its use as efficient metal-free catalyst for oxygen reduction

Controlled synthesis of graphene via electrochemical route and its use as efficient metal-free catalyst for oxygen reduction
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DOI:
10.1016/j.apcatb.2018.10.070
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发表时间:
2019-04-01
影响因子:
22.1
通讯作者:
Sun, Shuhui
Sun, Shuhui
中科院分区:
化学1区
文献类型:
--
作者:
Komba, Nathanael;Wei, Qiliang;Sun, Shuhui

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氧还原反应(ORR)是燃料电池运行中的关键步骤。探索高效、低成本和耐用的非贵重ORR催化剂以取代稀有和昂贵的Pt基催化剂,有望实现燃料电池的大规模商业化。在这里,我们报告了高质量的石墨烯(GP)的可控层的制造,使用一个简单的,通用的和具有成本效益的电化学剥离方法。我们的系统研究表明,石墨前体,电解质温度和热解条件在很大程度上影响石墨烯的层数和质量,从而对其ORR性能产生显着影响。将优化后的石墨烯样品在NH3气氛中进行热处理,得到氮掺杂石墨烯(N-GP)。作为一种无金属的电催化剂,N-GP表现出比GP更高的ORR活性,并且与最先进的Pt/C催化剂相当的ORR活性。此外,它还显示出比Pt/C催化剂在碱性溶液中更好的稳定性。
The oxygen reduction reaction (ORR) is a critical step in the operation of fuel cells. The exploration of efficient, low cost and durable non-precious ORR catalysts, to replace the rare and expensive Pt-based catalysts, is promising towards the large-scale commercialization of fuel cells. Here, we report the fabrication of high-quality graphene (GP) with controllable layers, using a simple, versatile and cost-effective electrochemical exfoliation method. Our systematic studies revealed that the graphite precursor, electrolyte temperature, and pyrolysis conditions largely affect the number of layers and quality of the graphene, which consequently has a significant effect on its ORR performance. The optimized graphene sample was subsequently heat-treated in the NH3 atmosphere to obtain the nitrogen-doped graphene (N-GP). As a metal-free electrocatalyst, N-GP exhibit much enhanced ORR activity than GP, and comparable ORR activity to the state-of-the-art Pt/C catalyst. Moreover, it also shows better stability than Pt/C catalyst in alkaline solution.