Collapse in crystalline structure and decline in catalytic activity of Pt nanoparticles on reducing particle size to 1 nm.
Collapse in crystalline structure and decline in catalytic activity of Pt nanoparticles on reducing particle size to 1 nm.
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DOI：
10.1021/ja076177b
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发表时间：
2007-11
影响因子：
15
通讯作者：
Yubao Sun;Zhuang Lin;Juntao Lu;Xinlin Hong;Peifang Liu
中科院分区：
文献类型：
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作者：
Yubao Sun;Zhuang Lin;Juntao Lu;Xinlin Hong;Peifang Liu
实验和计算相结合的研究表明，当Pt纳米颗粒的直径减小到1 nm时，晶体结构会自发地发生坍塌，由此引起的量子尺寸效应会导致氢氧化反应（HOR）的催化活性下降。分子动力学模拟证明了晶体结构向非晶态结构转变的合理性；通过密度泛函计算揭示了非晶态Pt纳米粒子的特殊电子结构。本研究不仅估计了Pt对HOR的利用极限，而且将Pt纳米颗粒对HOR的结构-活性关系扩展到很少触及的程度。
Combined experimental and computational studies show that, upon reducing the diameter of Pt nanoparticles down to 1 nm, a collapse in the crystalline structure occurs spontaneously and the thus-induced quantum size effect causes a decline in the catalytic activity toward hydrogen oxidation reaction (HOR). The conversion from crystalline to amorphous structure is rationalized by molecular dynamic simulations; and the special electronic structure of amorphous Pt nanoparticles is revealed via density functional calculations. Not only has the present work estimated the Pt utilization limit for HOR, but it also expands the structure−activity relationship of Pt nanoparticles toward HOR to an extent that has rarely been touched.