Local Platinum Environments in a Solid Analogue of the Molecular Periana Catalyst
Local Platinum Environments in a Solid Analogue of the Molecular Periana Catalyst
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DOI：
10.1021/acscatal.5b02305
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发表时间：
2016-03
期刊：
影响因子：
12.9
通讯作者：
Mario Soorholtz;L. Jones;D. Samuelis;C. Weidenthaler;Robin J. White;M. Titirici;D. Cullen;T. Zimmermann-T
中科院分区：
文献类型：
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作者：
Mario Soorholtz;L. Jones;D. Samuelis;C. Weidenthaler;Robin J. White;M. Titirici;D. Cullen;T. Zimmermann-T
通过在固体载体上引入活性物种来结合均相和多相催化的优点通常是提高催化剂整体性能的有效策略，尽管载体的影响通常是难以确定的，特别是在分子水平上。在这里，我们报道了共价三嗪骨架材料中铂物种的局部组成和结构，这是一种固体类似分子的Periana催化剂，在浓硫酸存在下，这两种催化剂都对甲烷的选择氧化具有活性。结合固体~(195)Pt核磁共振谱、像差校正扫描电子显微镜、X射线光电子能谱和X射线吸收光谱，观察到了铂-CTF和Periana催化剂的重要相似和不同之处，这可能与它们各自的宏观反应有关。
Combining advantages of homogeneous and heterogeneous catalysis by incorporating active species on a solid support is often an effective strategy for improving overall catalyst performance, although the influences of the support are generally challenging to establish, especially at a molecular level. Here, we report the local compositions, and structures of platinum species incorporated into covalent triazine framework (Pt-CTF) materials, a solid analogue of the molecular Periana catalyst, Pt(bpym)Cl2, both of which are active for the selective oxidation of methane in the presence of concentrated sulfuric acid. By using a combination of solid-state 195Pt nuclear magnetic resonance (NMR) spectroscopy, aberration-corrected scanning transmission electron microscopy (AC-STEM), X-ray photoelectron spectroscopy (XPS), and X-ray absorption spectroscopy (XAS), important similarities and differences are observed between the Pt-CTF and Periana catalysts, which are likely related to their respective macroscopic reac...