Strong Local Coordination Structure Effects on Subnanometer PtOx Clusters over CeO2 Nanowires Probed by Low-Temperature CO Oxidation
Strong Local Coordination Structure Effects on Subnanometer PtOx Clusters over CeO2 Nanowires Probed by Low-Temperature CO Oxidation
复制标题
低温 CO 氧化探测 CeO2 纳米线上亚纳米 PtOx 团簇的强局域配位结构效应
DOI：
10.1021/acscatal.5b00832
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发表时间：
2015-09-01
期刊：
影响因子：
12.9
通讯作者：
Zhang, Ya-Wen
中科院分区：
文献类型：
--
作者：
Ke, Jun;Zhu, Wei;Zhang, Ya-Wen
在分子水平上对负载型金属催化剂结构效应的基本理解对于开发广泛应用于工业的高性能催化剂是极其重要的，这是一个长期具有吸引力但又具有挑战性的多学科领域课题。在这项工作中，我们报道了局部配位结构对亚纳米PtOx簇在CeO2纳米线上作为探针反应在低温CO氧化中的催化活性的强烈影响。Pt原子和亚纳米团簇沉积形成PtOx的配位结构，并主要暴露（110）个面。在密度泛函理论模拟的辅助下，利用原位光谱实验深入研究了活性位点的反应性和PtOx位点的局部配位结构的变化。根据我们的观察，虽然在亚纳米尺度上高度分散的Pt位点可以提供更多的可接近性。
A fundamental understanding of the structural effects of supported metal catalysts at the molecular level is extremely important for developing high-performance catalysts that are widely used in industry, which is still a longstanding attractive but challenging topic in multidisciplinary fields. In this work, we report the strong effects of local coordination structures on the catalytic activity of subnanometric PtOx clusters over CeO2 nanowires in low-temperature CO oxidation as a probe reaction. Atoms and subnanometric clusters of Pt were deposited to form the coordination structure of PtOx on the well-defined CeO2 nanowires with mainly exposed (110) facets. The reactivity of active sites and the variation of the local coordination structures of the PtOx sites were deeply investigated with in situ spectroscopic experiments, assisted by density functional theory simulations. According to our observation, although the highly dispersed Pt sites at the subnanometric scale could provide increased accessible ...