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三维石油沥青基氮掺杂Mo_2C/碳骨架复合材料的构筑及析氢性能研究
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摘要
随着化石燃料的不断减少和全球温室效应的加剧,人类对清洁可再生能源需求的急迫性日益增强。氢气作为一种清洁的新能源,其众多优点吸引了大量研究者的高度关注,析氢反应(HER)更是成为了研究的重点。铂(Pt)基催化剂在析氢反应中具有较低的转换电位和优异的电流密度,但在地壳中的丰度和高昂的价格制约了其进一步的广范使用。碳化钼(Mo_2C)具有类Pt的催化活性,但商业化的Mo_2C由于其较大的微米尺寸使其析氢活性位点较少~([1])。通过调控其碳载体形貌和纳米尺寸上活性位的数量有望得到性能优异的HER催化剂~([2])。本文从廉价且富含芳香分的石油沥青出发,温和条件下制备出一种三维沥青基氮掺杂Mo_2C/碳骨架复合材料(3D Mo_2C-NCF)。通过催化性能测试,3D Mo_2C-NCF在HER过程中的起始电位接近75 mV,电流密度10 mV/cm~2时的过电位为-190mV,相比于无沥青体系表现出更优异的催化活性。本研究在制备新型非铂析氢催化剂的同时,为重质油的高附加值利用提供了新的途径。
Although Pt-based catalysts are efficient hydrogen evolution reaction(HER) catalysts with high current density at low overpotential, the low content in the earth and high price of Pt restrict its further large-scale application. Owing to the similar catalytic activities to that of Pt, Mo_2C has been expected to be an effective non-Pt electrocatalyst for HER. The nano active sites and electric conductivity of Mo_2C are key parameters for high activity. Petroleum asphalt with enriched aromatic hydrocarbon was used as raw material to obtain the three dimensional Mo_2C/N-doped carbon framework hybrid(3D Mo_2C-NCF). The as-made Mo_2C-NCF shows remarkable HER catalytic activity, including small overpotential(75mV), large cathodic current density. This work can bring us a kind of highly active catalyst without Pt for HER. Meanwhile, it can pave a way for the high-valued utilization of petroleum asphalt.
引文
[1]Liu,Y;Yu,G;Li,G D;Sun,Y H.Angew.Chem.Int.Ed.,2015,54(37):10752.
    [2]Zou,X;Zhang,Y.Chem.Soc.Rev.,2015,44(15):5148.

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