高活性氧还原纳米电催化剂的研究
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摘要
高活性、低成本氧还原催化剂及其催化活性机理的研究对于燃料电池及金属空气电池的发展至关重要。本报告将讨论我们最近在如何设计高活性氧还原催化活性位点、提高活性位数量及催化活性机理方面的最新研究进展~(1-7)。不仅通过纳米结构化催化剂的设计获得了高活性的低成本氧还原催化剂,而且深入研究了所发展的高活性Fe-N-C催化剂的催化活性机理。通过系列先进表征技术、对比实验与理论计算,表明碳层包覆的金属态Fe基纳米晶体/团簇促进了相邻Fe-N_x位点的氧还原活性是这类Fe-N-C催化剂高活性的重要原因。
In this presentation, several reasonable ways for designing new low-cost nanocatalysts with high electrocatalytic activities and superior stability for ORR will be discussed. By focusing on the creation and the enrichment of highly active sites for ORR and simultaneously considering the mass transfer and electron transportation, we have developed several efficient ORR nanocatalysts.1-7 Furthermore, understanding the origin of high activity of these electrocatalysts in ORR is also critical for developing efficient non-precious metal catalysts but still challenging. We developed a new highly active Fe-N-C ORR catalyst containing Fe-Nx coordination sites and Fe/Fe_3C nanocrystals, and revealed the origin of its activity by intensively investigating the composition and the structure of the catalyst and their correlations with the electrochemical performance. Based on our experimental and theoretical results, it can be concluded that the high ORR activity in this type of Fe-N-C catalysts should be ascribed to that Fe/Fe_3C nanocrystals boost the activity of Fe-N_x. These new findings open an avenue for the rational design and bottom-up synthesis of low-cost highly active ORR electrocatalysts.
引文
[1]W.J.Jiang,J.S.Hu,X.Zhang,Y.Jiang,B.B.Yu,Z.D.Wei,L.J.Wan,J.Mater.Chem.A.2014,2:10154.
    [2]R.J.Huo,W.J.Jiang,S.L.Xu,F.Z.Zhang,J.S.Hu,Nanoscale,2014,6:203.
    [3]Y.Zhang,W.J.Jiang,X.Zhang,L.Guo,J.S.Hu,Z.D.Wei,L.J.Wan,Phys.Chem.Chem.Phys.,2014,6:13605.
    [4]L.Guo,W.J.Jiang,Y.Zhang,J.S.Hu,Z.D.Wei,L.J.Wan,ACS Catal.,2015,5:2903.
    [5]Y.Zhang,W.J.Jiang,X.Zhang,L.Guo,J.S.Hu,Z.D.Wei,L.J.Wan,ACS Appl.Mater.Interfaces,2015,7:11508.
    [6]Y.Zhang,W.J.Jiang,X.Zhang,L.Guo,J.S.Hu,Z.D.Wei,L.J.Wan,J.Mater.Chem.A.2016,DOI:10.1039/C6TA01655C.
    [7]W.J.Jiang,L.Gu,L.Li,Y.Zhang,X.Zhang,L.J.Zhang,J.Q.Wang,J.S.Hu,Z.D.Wei,L.J.Wan,J.Am.Chem.Soc.,2016,138:3570.

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