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首页> 外文期刊>Advanced energy materials >Controlling the Active Sites of Sulfur-Doped Carbon Nanotube-Graphene Nanolobes for Highly Efficient Oxygen Evolution and Reduction Catalysis
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Controlling the Active Sites of Sulfur-Doped Carbon Nanotube-Graphene Nanolobes for Highly Efficient Oxygen Evolution and Reduction Catalysis

机译：控制硫掺杂碳纳米管 - 石墨烯纳米纳米的活性位点，用于高效氧气进化和还原催化

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摘要

Controlling active sites of metal-free catalysts is an important strategy to enhance activity of the oxygen evolution reaction (OER). Many attempts have been made to develop metal-free catalysts, but the lack of understanding of active-sites at the atomic-level has slowed the design of highly active and stable metal-free catalysts. A sequential two-step strategy to dope sulfur into carbon nanotube-graphene nanolobes is developed. This bidoping strategy introduces stable sulfur-carbon active-sites. Fluorescence emission of the sulfur K-edge by X-ray absorption near edge spectroscopy (XANES) and scanning transmission electron microscopy electron energy loss spectroscopy (STEM-EELS) mapping and spectra confirm that increasing the incorporation of heterocyclic sulfur into the carbon ring of CNTs not only enhances OER activity with an overpotential of 350 mV at a current density of 10 mA cm(-2), but also retains 100% of stability after 75 h. The bidoped sulfur carbon nanotube-graphene nanolobes behave like the state-of-the-art catalysts for OER but outperform those systems in terms of turnover frequency (TOF) which is two orders of magnitude greater than (20% Ir/C) at 400 mV overpotential with very high mass activity 1000 mA cm(-2) at 570 mV. Moreover, the sulfur bidoping strategy shows high catalytic activity for the oxygen reduction reaction (ORR). Stable bifunctional (ORR and OER) catalysts are low cost, and light-weight bidoped sulfur carbon nanotubes are potential candidates for next-generation metal-free regenerative fuel cells.
机译：控制无金属催化剂的活性位点是增强氧气进化反应（oer）活性的重要策略。已经制定了许多尝试来开发无金属催化剂，但对原子水平的活性位点缺乏了解，从而减缓了高活性和稳定的无金属催化剂的设计。开发了将硫磺掺入碳纳米管 - 石墨烯纳米烯醛铅的序贯两步策略。这种潮流策略介绍了稳定的硫磺碳活性位点。通过X射线吸收附近边缘光谱（XANES）和扫描透射电子显微镜电子能量损失光谱（STEM-EEL）测绘和光谱通过X射线吸收的荧光发射确认，增加杂环硫的掺入CNT的碳环。不仅在10 mA cm（-2）的电流密度为350mV的过电位而增强了Oer活动，而且还保留了75小时后的100％稳定性。硫磺碳纳米管 - 石墨烯纳米甲烯纳米表现得像oer的最先进的催化剂，但在周转频率（TOF）方面优于这些系统，这是400的两个数量级大于（20％IR / C） MV超势，在570 mV下具有非常高的质量活性1000 mA cm（-2）。此外，硫均匀策略显示出用于氧还原反应（ORR）的高催化活性。稳定的双官能（ORR和OER）催化剂是低成本，并且轻掺杂的硫碳纳米管是下一代无金属再生燃料电池的潜在候选者。

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