具有低Pd-Au负载的氧化倾向银基纳米颗粒用于碱性介质中乙醇和甘油电氧化
Oxophilic Silver-Based Nanoparticles with Low Pd-Au Loading for Ethanol and Glycerol Electrooxidation in Alkaline Media
AI总结：
研究了氧化倾向银纳米颗粒与少量Pd和Au的电催化活性，用于碱性介质中乙醇和甘油氧化反应，发现AgPd/C和AgPdAu/C催化剂在乙醇氧化反应中表现出更小的电流密度和更负的起始电位，且具有更高的耐久性。
摘要：
本文研究了氧化倾向银纳米颗粒与少量Pd和Au的电催化活性，用于碱性介质中乙醇氧化反应（EOR）和甘油氧化反应（GOR）。EOR和GOR结果表明，AgPd/C和AgPdAu/C电催化剂（含5 wt% Pd）相比商业Pd/C催化剂（含20 wt% Pd）表现出竞争性电流密度和更负的起始电位。在EOR过程中，原位FTIR分析证实乙醇首先吸附为乙酰化物种，随后氧化为乙酸根离子，是碱性介质中的主要稳定产物。然而，Pd和Au的掺入并未显著改变反应机制。在GOR中，原位FTIR研究显示催化剂组成影响氧化路径：Pd丰富的表面促进草酸盐形成，而Ag的显著存在促进更深入的氧化（至碳酸盐），AgPdAu三元催化剂表现出中间行为。一个关键优势是Ag对反应产物不可逆吸附的低敏感性，从而提高电催化剂的耐久性。因此，高电位下Ag的表面偏析可修改催化表面反应性，影响稳定性和效率。
英文摘要：
The electrocatalytic activity of oxophilic Ag nanoparticles, combined with small amounts of Pd and Au, was investigated for ethanol oxidation reactions (EOR) and glycerol oxidation reactions (GOR) in alkaline media. The EOR and GOR results revealed competitive current densities and less positive onset potentials for the AgPd/C and AgPdAu/C electrocatalysts, both containing 5 wt% Pd, compared to the commercial Pd/C catalyst, which has a significantly higher loading of the costly noble metal (20 wt%). In situ FTIR analyses during EOR confirmed that ethanol is initially adsorbed as acetylated species, which are subsequently oxidized to acetate ions, the main stable product in alkaline medium. However, the incorporation of Pd and Au into the Ag matrix did not significantly alter the reaction mechanism. During GOR, the in situ FTIR studies demonstrated that catalyst composition influences the oxidation pathways: Pd-rich surfaces favor oxalate formation, while a significant presence of Ag promotes deeper oxidation (up to carbonate), with the AgPdAu ternary catalyst exhibiting intermediate behavior. One key benefit is the lower susceptibility of Ag to irreversible adsorption of reaction byproducts, which enhances electrocatalyst durability. Thus, surface segregation of Ag at high potentials can modify the catalytic surface reactivity, affecting both stability and efficiency.
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