Ethanol oxidation on shape-controlled platinum nanoparticles at different pHs: A combined in situ IR spectroscopy and online mass spectrometry study
Ethanol oxidation on shape-controlled platinum nanoparticles at different pHs: A combined in situ IR spectroscopy and online mass spectrometry study
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DOI：
10.1016/j.jelechem.2015.12.034
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发表时间：
2016-02-15
影响因子：
4.5
通讯作者：
Feliu, Juan M.
中科院分区：
文献类型：
--
作者：
Buso-Rogero, Carlos;Brimaud, Sylvain;Feliu, Juan M.
利用电化学、衰减全反射傅里叶变换红外光谱(ATR-FTIR)，特别是差示电化学质谱(DEM)技术研究了不同形状控制的铂纳米颗粒在不同pH值下的乙醇氧化反应，后者提供了乙醇氧化产物的有趣的定量信息。为此，使用了两个铂纳米颗粒样品：(100)和(111)择优取向。铂纳米粒子。研究结果与前人的研究结果一致，即优先分解产物取决于表面结构，Coads形成在(100)域上，乙醛/醋酸生成在(111)域上。然而，有关低电位下CHX和CO生成随pH变化的新信息表明，CHX的生成有利于CO在(100)结构域上吸附的减少。在较高的电位下，CHX和CO片段都会完全氧化成二氧化碳。在(111)Pt纳米粒子中，C-C键的断裂受到阻碍，即使在0.5M的H_2SO_4中也有利于乙醛和乙酸酯的形成。当pH升高时，CL碎片变得更少，在所研究的最高pH下几乎可以忽略不计。(C)2015爱思唯尔B.V.保留所有权利。
Ethanol oxidation on different shape-controlled platinum nanoparticles at different pHs was studied using electrochemical, Attenuated Total Reflection-Fourier Transform Infrared Spectroscopy (ATR-FTIR) and, especially, Differential Electrochemical Mass Spectrometry (DEMS) techniques, the latter giving interesting quantitative information about the products of ethanol oxidation. Two Pt nanoparticle samples were used for this purpose: (100) and (111) preferentially oriented. Pt nanoparticles. The results are in agreement with previous findings that the preferred decomposition product depends on surface structure, with COads formation on (100) domains and acetaldehyde/acetic acid formation on (111) domains. However, new information has been obtained about the changes in CHx and CO formation at lower potentials when the pH is changed, showing that CHx formation is favored against the decrease in CO adsorption on (100) domains. At higher potentials, complete oxidation to CO2 occurs from both CHx and CO fragments. In (111) Pt nanoparticles, the splitting of C-C bond is hindered, favoring acetaldehyde and acetate formation even in 0.5 M H2SO4. Cl fragments become even less when the pH increases, being nearly negligible in the highest pH studied. (C) 2015 Elsevier B.V. All rights reserved.