Sinter‐Resistant Platinum Catalyst Supported by Metal–Organic Framework,Angewandte Chemie International Edition

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Sinter‐Resistant Platinum Catalyst Supported by Metal–Organic Framework
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-01-02 , DOI: 10.1002/anie.201708092
In Soo Kim _{1,

2} , Zhanyong Li ₃ , Jian Zheng ₄ , Ana E. Platero-Prats ₅ , Andreas Mavrandonakis ₆ , Steven Pellizzeri ₇ , Magali Ferrandon ₈ , Aleksei Vjunov ₄ , Leighanne C. Gallington ₅ , Thomas E. Webber ₆ , Nicolaas A. Vermeulen ₃ , R. Lee Penn ₆ , Rachel B. Getman ₇ , Christopher J. Cramer ₆ , Karena W. Chapman ₅ , Donald M. Camaioni ₄ , John L. Fulton ₄ , Johannes A. Lercher _{4,

9} , Omar K. Farha ₃ , Joseph T. Hupp _{1,

3} , Alex B. F. Martinson ₁

Affiliation

Single atoms and few‐atom clusters of platinum are uniformly installed on the zirconia nodes of a metal‐organic framework (MOF) NU‐1000 via targeted vapor‐phase synthesis. The catalytic Pt clusters, site‐isolated by organic linkers, are shown to exhibit high catalytic activity for ethylene hydrogenation while exhibiting resistance to sintering up to 200 °C. In situ IR spectroscopy reveals the presence of both single atoms and few‐atom clusters that depend upon synthesis conditions. Operando X‐ray absorption spectroscopy and X‐ray pair distribution analyses reveal unique changes in chemical bonding environment and cluster size stability while on stream. Density functional theory calculations elucidate a favorable reaction pathway for ethylene hydrogenation with the novel catalyst. These results provide evidence that atomic layer deposition (ALD) in MOFs is a versatile approach to the rational synthesis of size‐selected clusters, including noble metals, on a high surface area support.

中文翻译：

金属有机框架支持的抗烧结铂催化剂

通过目标气相合成将铂的单原子和少数原子簇均匀地安装在金属-有机骨架（MOF）NU-1000的氧化锆节点上。通过有机连接基位点隔离的催化Pt团簇显示出对乙烯加氢的高催化活性，同时对高达200°C的烧结具有抵抗力。原位红外光谱揭示了取决于合成条件的单个原子和少数原子团簇的存在。Operando X射线吸收光谱和X射线对分布分析揭示了在生产过程中化学键合环境和簇尺寸稳定性的独特变化。密度泛函理论计算阐明了用新型催化剂进行乙烯加氢的有利反应途径。

更新日期：2018-01-02

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