二维纳米结构氧还原催化材料的制备与性能
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摘要
经过十几年来对以石墨烯为代表的二维材料的研究,纳米片层结构材料的合成和应用有了极大的发展~([1][2])。然而,组成单一的二维材料无法满足现代技术和应用对性质可调的材料的需求。我们采用不同的方法合成了多种二维结构复合与元素化学掺杂材料,以期替代Pt基氧还原反应(ORR)催化材料,这些新型二维材料包括:氮掺杂石墨烯负载Fe_3C纳米复合物(Fe_3C/NGr)、氮掺杂石墨烯负载超小MoC纳米复合物(MoC/NGr)、P掺杂MoS_2超薄纳米片层材料(P-MoS_2)以及O边缘取代的超薄MoS_2片层材料(O-MoS_2)。在碱性条件下,系统研究了Fe_3C/NGr、MoC/NGr、P-MoS_2和O-MoS_2材料的ORR催化性能,通过改变合成条件,优化了材料的催化性能,并结合物理表征初步探讨了催化反应机理。研究发现,在碱性条件下,这些材料均表现出良好的ORR催化活性,具有良好的四电子选择性。功能化NGR和MoS_2纳米片层材料因高储量、低成本以及高ORR催化活性,有望在燃料电池和金属空气电池中有潜在的应用前景。
In decades, graphene has attracted growing research interest, leading to a great development of synthesis and application of 2D materials ~([1])~([2]). However, 2D materials with single component are hard to satisfy the requirement of properties versatility for modern technological applications. Herein, several types of functionalized 2D nanosheets, including Fe_3C/NGr, Mo C/NGr, P-MoS_2 and O-MoS_2, were achieved by heteroatom doping and one-step combination, and demonstrated as efficient cathode ORR catalysts to instead of the Pt-based catalyst. The ORR catalytic performances of Fe_3C/NGr, Mo C/NGr, P-MoS_2 and O-MoS_2 in alkaline media were studied in detail. The optimal catalytic performance has been achieved via tuning the reaction conditions, and the catalytic activity mechanism has been discussed preliminary. The proposed catalysts display much improved ORR catalytic performances in alkaline media with good four-electron selectivity. The as-prepared functionalized NGR and MoS_2 nanosheets are promising ORR catalytic materials in fuel cells and metal-air batteries.
引文
[1]Novoselov,K.S.;Geim,A.K.;Morozov,S.V.;Jiang,D.;Zhang,Y.;Dubonos,S.V.;Grigorieva,I.V.;Firsov,A.A.,Science 2004,306:666.
    [2]Lee,C.;Yan,H.;Brus,L.E.;Heinz,T.F.;Hone,J.;Ryu,S.,Acs Nano 2010,4:2695.

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