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富氮聚合物衍生碳材料的制备及其氧还原催化性能研究
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摘要
廉价且高活性的氧还原电催化剂对燃料电池和金属空气电池的工业化应用起到至关重要的作用。1-5由于其可调控的外层电子和自旋结构,异质原子掺杂碳材料作为氧还原催化剂被广泛地研究,且其活性和稳定性已经接近于贵金属铂基材料。在本文中,我们报道了一系列基于富氮聚合物衍生的异质原子掺杂碳材料,它们具有高密度金属位点以及高比表面积。研究结果表明富氮聚合物为前驱体制备的异质原子掺杂碳材料的氧还原活性远高于常规低氮聚合物制备的碳材料氧还原催化活性。在酸性和碱性电解质体系中,其氧还原催化性能接近甚至超越了贵金属铂基材料的活性,其高催化活性来源于高密度金属活性位点和高比表面积。
Cost-effective and highly-performance oxygen reduction reaction(ORR) electrocatalysts are essential for the industrial application of various types of fuel cells and metal-air batteries. Carbon materials co-doped with nitrogen and transition metals(M-N_x/C) have been widely studied as ORR catalysts because of their tunable electronic and spin structure in outer orbital, and advanced ORR activity and stability that resemble those of Pt-based precious metal catalysts. In this study, we report a series of M-N_x/C materials with dense metal sites and high surface area by using nitrogen-rich polymers as the starting precursors. The results indicated that the ORR activity of M-N_x/C materials was substantially promoted by using nitrogen-rich polymer precursors compared with that those of general nitrogen-contained polymers. The newly-developed M-N_x/C catalysts exhibited comparable ORR activity to that of commercial Pt/C catalysts in the alkaline and acidic medium, respectively.
引文
[1]Zhao,Y.;Watanabe,K.;Hashimoto,K.J.Am.Chem.Soc.2012,134,19528.
    [2]Zhao,Y.;Watanabe,K.;Hashimoto,K.J.Mater.Chem.2012,22,12263.
    [3]Zhao,Y.;Watanabe,K.;Hashimoto,K.J Mater Chem A 2013,1,1450.
    [4]Zhao,Y.;Nakamura,R.;Kamiya,K.;Nakanishi,S.;Hashimoto,K.Nat.Commun.2013,4.
    [5]Zhao,Y.;Kamiya,K.;Hashimoto,K.;Nakanishi,S.J.Mater.Chem.A 2016,4,3858.

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