Atomic Layer Deposition in a Metal–Organic Framework: Synthesis, Characterization, and Performance of a Solid Acid

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• 作者：Martino RimoldiVarinia Bernales ; Joshua Borycz ; Aleksei Vjunov ; Leighanne C. Gallington ; Ana E. Platero-PratsI. S. Kim ; John L. FultonA. B. F. Martinson ; Johannes A. Lercher ; Karena W. Chapman ; Christopher J. Cramer ; Laura GagliardiJoseph T. Hupp ; Omar K. Farha
• 刊名：Chemistry of Materials
• 出版年：2017
• 出版时间：February 14, 2017
• 年：2017
• 卷：29
• 期：3
• 页码：1058-1068
• 全文大小：752K
• ISSN：1520-5002

文摘

NU-1000, a zirconium-based metal–organic framework (MOF) featuring mesoporous channels, has been postsynthetically metalated via atomic layer deposition in a MOF (AIM) employing dimethylaluminum iso-propoxide ([AlMe₂OⁱPr]₂, DMAI), a milder precursor than widely used trimethylaluminum (AlMe₃, TMA). The aluminum-modified NU-1000 (Al-NU-1000) has been characterized with a comprehensive suite of techniques that points to the formation of aluminum oxide clusters well dispersed through the framework and stabilized by confinement within small pores intrinsic to the NU-1000 structure. Experimental evidence allows for identification of spectroscopic similarities between Al-NU-1000 and γ-Al₂O₃. Density functional theory modeling provides structures and simulated spectra, the relevance of which can be assessed via comparison to experimental IR and EXAFS data. The catalytic performance of Al-NU-1000 has been benchmarked against γ-Al₂O₃, with promising results in terms of selectivity.