多孔碳负载PtM的制备及其电催化性能研究
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摘要
化石燃料供应不足和环境污染的双重压力使燃料电池备受关注。催化剂的高成本、低寿命是制约其商品化的关键。本工作以多孔碳为碳源,以H2PtC l6和过渡金属盐MClx为前躯体,通过气相加氢还原的方法制备出多孔碳负载的PtM(M=Bi,Ni,Co)纳米电催化剂。进一步地根据具体研究体系的需要,通过控制热处理的温度、时间和环境气氛(H2,Ar,或Air),调控所制备电催化剂的表面组成,调控出核为中间相金属间化合物,壳为M表面富集或Pt表面富集的PtM纳米催化剂。XRD和STEM表征知该材料为中间相金属间化合物,并具有相应的壳层结构。以CO和甲酸为分子探针,用循环伏安法和电化学原位红外光谱法验证了催化剂的表面组成。将PtM催化剂分别用于甲酸氧化和氧还原反应(ORR),发现Pt表面富集的PtM/PC对ORR具有很高的活性和稳定性,而M表面富集的PtM/PC对甲酸具有很高的催化活性。本工作提出的控制热处理方法可重现性好,易于操作,可实现特定反应体系纳米电催化剂的宏量合成。
Both supply shortage in fossil fuels and environmental hazard raised concern over the development of fuel cell. However, the high cost and short life of catalysts impose technical restrictions on the commercialization of fuel cell. In this work, we developed a controlled thermal treatment method(CTTM) to synthesize the PtM intermetallic with the M-rich or Pt-skin, on the porous graphitic carbon(PtM/PC). Based on the results of CV, CO stripping and line-profile analysis using STEM/energy dispersive spectroscopy(EDS), we may confirm the surface composition of PtM. This PtM intermetallic with M-rich showed extremely high mass activity and stability towards oxidizing of formic acid; and PtM /PC with Pt-skin structure has a great activity and durability to ORR. The synthesis method of PtM /PC is simple and reproducible, and can be readily scaled up to produce high-performance electrocatalysts, and can be generalized toward the design of other multimetallic systems.
引文
[1]Zhang B.W.;Zhang Z.C.;Liao H.G.;Gong Y.;Gu L.;Qu X.M.;You L.X.;Liu S.;Huang L.;Tian X.C.;Huang R.;Zhu F.C.;Liu T.;Jiang Y.X.;Zhou Z.Y.;Sun S.G.,Nano Energy,2016,19:198.

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