Ethanol chemisorption on core–shell Pt-nanoparticles: an ab initio study
Ethanol chemisorption on core–shell Pt-nanoparticles: an ab initio study
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核壳 Pt 纳米颗粒上的乙醇化学吸附：从头开始研究
DOI：
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发表时间：
2018
期刊：
影响因子：
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通讯作者：
F. Baletto
中科院分区：
文献类型：
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作者：
V. A. Rigo;C. R. Miranda;F. Baletto
摘要
通过从头计算，我们研究了乙醇在分离二元纳米合金（NAs）上的化学吸附性质。我们选择具有55个原子的二十面体形状的纳米结构，其中Pt最外层在M-核心上，M = Ag，Pd，Ni。相对于具有相同组成的纳米膜，乙醇结合能增加。这不仅仅是由于观察到的Pt-O距离的缩短，而是取决于乙醇吸附后的纳米颗粒变形。纳米颗粒内的这种几何变形可以解释为径向呼吸，其对吸附位点敏感，通过O-锚点和乙基的相对位置来识别。更有趣的是，在Pd@Pt中较大且在Ni@Pt中较小的核依赖性，其涉及从乙醇和M-核向Pt-壳的有效电子转移。在这个新的分析的观点，Pd@Pt NAs显示出最有前途的乙醇氧化的功能。
图形摘要
Abstract
By means of ab initio calculations, we have investigated the chemisorption properties of ethanol onto segregating binary nanoalloys (NAs). We select nanostructures with icosahedral shape of 55 atoms with a Pt outermost layer over an M-core with M = Ag, Pd, Ni. With respect to nanofilms with equivalent composition, there is an increase of the ethanol binding energy. This is not merely due to observed shortening of the Pt–O distance but depends on the nanoparticle distortion after ethanol adsorption. This geometrical distortion within the nanoparticle can be interpreted as a radial breathing, which is sensitive to the adsorption site, identified by the O-anchor point and the relative positions of the ethyl group. More interestingly, being core-dependent larger in Pd@Pt and smaller in Ni@Pt, it relates to an effective electron transfer from ethanol and the M-core towards the Pt-shell. On the view of this new analysis, Pd@Pt NAs show the most promising features for ethanol oxidation.
Graphical abstract
影响因子：
10.8
作者：
Di Paola, Cono;D'Agosta, Roberto;Baletto, Francesca
通讯作者：
Baletto, Francesca