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Pt-Pd alloy nanoparticle-decorated carbon nanotubes: A durable and methanol tolerant oxygen reduction electrocatalyst

机译:Pt-Pd合金纳米粒子修饰的碳纳米管:耐甲醇耐久的持久性氧还原电催化剂

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We describe the decoration of multiwalled carbon nanotubes (MCNTs) with Pt-Pd alloy nanoelectrocatalysts of three different compositions and their electrocatalytic performance toward the oxygen reduction reaction (ORR). The decoration of the MCNTs involves polymer-assisted impregnation of metal precursors PtCl _6 ~(2-) and PdCl _4 ~(2-) and the subsequent reduction of the impregnated precursors by a modified polyol route. The composition of the catalyst was controlled by tuning the molar ratio of the precursors during their impregnation. Electron probe microscopic analysis shows that the catalysts have compositions of Pt _(46)Pd _(54); Pt _(64)Pd _(36) and Pt _(28)Pd _(72). The Pt _(46)Pd _(54) and Pt _(64)Pd _(36) catalysts have truncated octahedral and icosahedral shapes with a size ranging from 8 to 10 nm. On the other hand, the catalyst of Pt _(28)Pd _(72) composition has a spherical/quasispherical shape with a size distribution of 1 2 nm. The XPS measurement confirms the signature of metallic Pt and Pd. The Pt _(46)Pd _(54) catalyst has a pronounced electrocatalytic activity toward the ORR with a specific and mass activity of 378 μcm ~(-2) _(Pt Pd) and 64 μA μg ~(-1) _(PtPd), respectively at 0.8 V. Moreover, the Pt _(46)Pd _(54) nanoelectrocatalyst is highly durable and it retains its initial catalytic activity even after 1000 extensive cycles. Interestingly, this catalyst has a very high tolerance toward methanol and it does not favor the oxidation of methanol in the potential window of 0.11.4 V. The electrocatalytic activity of the alloy electrocatalyst is compared with commercially available Pt black and MCNT-supported spherical Pt nanoparticles. The catalytic activity of the Pt _(46)Pd _(54) nanoelectrocatalyst is higher than the other catalysts. The Pt _(46)Pd _(54) catalyst outperforms the electrocatalytic activity of all other catalysts.
机译:我们描述了三种不同组成的Pt-Pd合金纳米电催化剂对多壁碳纳米管(MCNTs)的装饰及其对氧还原反应(ORR)的电催化性能。 MCNT的装饰涉及金属前体PtCl _6〜(2-)和PdCl _4〜(2-)的聚合物辅助浸渍,以及随后通过改性的多元醇途径还原浸渍的前体。通过调节前体在浸渍过程中的摩尔比来控制催化剂的组成。电子探针显微镜分析表明,该催化剂的组成为Pt_(46)Pd_(54)。 Pt _(64)Pd _(36)和Pt _(28)Pd _(72)。 Pt_(46)Pd_(54)和Pt_(64)Pd_(36)催化剂具有截短的八面体和二十面体形状,尺寸范围为8至10 nm。另一方面,Pt_(28)Pd_(72)组成的催化剂具有球形/准球形形状,其尺寸分布为1 2 nm。 XPS测量证实了金属Pt和Pd的签名。 Pt_(46)Pd_(54)催化剂对ORR具有明显的电催化活性,比活性和质量活度分别为378μcm〜(-2)_(Pt Pd)和64μAμg〜(-1)_( PtPd)分别为0.8V。此外,Pt _(46)Pd _(54)纳米电催化剂具有很高的耐久性,即使经过1000个大循环也能保持其初始催化活性。有趣的是,该催化剂对甲醇具有很高的耐受性,并且不利于甲醇在0.11.4 V的电势窗口中氧化。将合金电催化剂的电催化活性与市售Pt黑和MCNT负载的球形Pt进行了比较。纳米粒子。 Pt_(46)Pd_(54)纳米电催化剂的催化活性高于其他催化剂。 Pt_(46)Pd_(54)催化剂的性能优于所有其他催化剂。

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