On the structural origin of the catalytic properties of inherently strained ultrasmall decahedral gold nanoparticles.
On the structural origin of the catalytic properties of inherently strained ultrasmall decahedral gold nanoparticles.
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DOI：
10.1021/nl300067q
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发表时间：
2012-03
期刊：
影响因子：
10.8
通讯作者：
M. Walsh;Kenta Yoshida;A. Kuwabara;Mungo Pay;P. Gai;E. Boyes
中科院分区：
文献类型：
--
作者：
M. Walsh;Kenta Yoshida;A. Kuwabara;Mungo Pay;P. Gai;E. Boyes
多层孪晶金纳米粒子固有的应变结构导致其反应活性的新机制为小颗粒金纳米粒子令人惊讶的催化活性提供了进一步的解释。原子缺陷结构的表面应变研究和十面体结构中原子柱位移的定量分析通过像差校正透射电镜观察到，表面最近邻距离的平均膨胀为5.6%，其中许多应变超过10%。密度泛函理论计算得到的修改金d带状态预测一氧化碳氧化活性显著增强。这些新发现对纳米颗粒在化学工艺技术中的应用具有重要意义，包括多相催化。
A new mechanism for reactivity of multiply twinned gold nanoparticles resulting from their inherently strained structure provides a further explanation of the surprising catalytic activity of small gold nanoparticles. Atomic defect structural studies of surface strains and quantitative analysis of atomic column displacements in the decahedral structure observed by aberration corrected transmission electron microscopy reveal an average expansion of surface nearest neighbor distances of 5.6%, with many strained by more than 10%. Density functional theory calculations of the resulting modified gold d-band states predict significantly enhanced activity for carbon monoxide oxidation. The new insights have important implications for the applications of nanoparticles in chemical process technology, including for heterogeneous catalysis.