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氮掺杂石油焦基碳量子点的高效制备及其电催化析氢性能
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摘要
石油焦是石油炼制的副产物,量大价廉且含碳量高,灰分等杂质相对较少,是制备碳质材料的优质原料,开发石油焦基功能化碳材料是实现其高附加值利用的重要途径之一。碳量子点(Carbon Quantum Dots,CQDs)具有粒径小、比表面积大、官能团丰富、电子传导快等特点,在生物成像、药物传输、离子及分子检测等方面的应用已取较大进展。CQDs/MoS_2复合物已用于光诱导电催化析氢(HER),但其作用机理及应用价值还有待于深入研究。本文以石油焦为碳源,采用电化学氧化法,一步制得氮掺杂石油焦基CQDs。该法无需进行透析除盐纯化,高效环保且产品收率高达20%。所制N-CQDs表面含有大量含氮及含氧基团,易与其他化合物高效结合,在促进电子传输的同时可增加催化活性位点数目,增大催化剂有效作用面积。基于N-CQDs设计合成的CQDs/Ni_3S_2/NF(Nifoam,NF)复合型HER催化剂,在1 M KOH中电流密度高达150mA·cm~(-2),电流密度为10 mA·cm~(-2)时,过电位为-210 mV,在电催化析氢领域具有很好的应用前景。
Petroleum coke with high content of carbon and low content of ash is a by-product in oil refining process. As the increasing heavy component in crude oil, the development of petroleum coke-based functionalized carbon materials has become an important method to realize high value-added utilization of heavy oil. Here we report a one-step electrochemical oxidation method to prepare nitrogen-doped petroleum coke-based carbon quantum dots(CQDs), without further dialysis and purification, and the product yield reached up to 20%. CQDs/Ni_3S_2/NF was designed for high-performance binder-free catalyst for electrocatalytic hydrogen evolution, featured by a geometrical catalytic current density of 10 mA ·cm~(-2) at an overpotential of -210 mV in 1 M KOH, with outstanding long-term operational stability. The as-made CQDs/Ni_3S-2/NF has a good application future in the field of hydrogen evolution reaction(HER).
引文
[1]Wu,M.B.;Wang,Y.;Wu,W.T.;Hu,C;et al.Carbon,2014,78:480.
    [2]Lim,S.Y.;Shen,W.;Gao,Z.Chem.Soc.Rev.,2015,44:362.
    [3]Zhao,S.Y.;Li,C.X.;Wang,L.P.;Liu,N.Y;et al.Carbon,2016,99:599.

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