碳载Au上Pt类单层的CO辅助沉积及对碱性乙醇氧化的电催化
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摘要
乙醇燃料电池具有燃料绿色可再生、理论能量密度高等优点,但乙醇电氧化动力学迟缓、质量活性待提高等问题限制了铂基催化剂的应用。因此,简便合成具有高质量活性的铂基催化剂,并阐明其提高电催化乙醇氧化活性的机理具有重要意义。在诸多相关研究中,通过欠电位沉积-置换方式在金上形成Au@Pt-q ML准单层结构,可提升乙醇电氧化活性[1],但上述借助外界电位的方法难以放量制备。最近我们利用CO分子对Pt(II)的还原性及形成络合物的能力,实现了Au@Pt-q ML/C的液相法可控制备,所得Au@Pt-q ML/C对碱性介质乙醇电催化反应具有极佳的活性[2]。我们还利用原位红外光谱手段揭示了相关电催化过程反应中间体和产物的生成、消耗及吸脱附随电位、时间变化行为。
Owing to limited reserve and high cost of Pt, one of the most adopted strategies is to develop high performance Pt-based catalysts with high mass activity. Pt quasi monolayer(Pt-q ML) on Au promotes electro-catalytic oxidation of ethanol and the Pt-q ML possesses the highest atomic utilization. To replace the external-electricity required UPD-Galvanic Replacement method and to facilitate scale-up synthesis of Au@Pt-q ML/C, we have developed a facile electroless deposition of Pt-q ML on Au/C by using CO as both reducing and capping agents. Compared to Pt/C, the as-formed Au@Pt-ML/C shows a total metal mass activity 5 times as high towards ethanol oxidation in alkaline media. In situ FTIR has been applied to provide a mechanistic understanding of the electrocatalytic process.
引文
[1]Li,M.;Liu,P.;Adzic,R.R.J.Phys.Chem.Lett.2012,3:3480.
    [2]Wang,H;Jiang,K;Chen Q.L.;Xie,Z.X.;Cai,W.B.Chem.Commun.2016,52:374.

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