期刊
INORGANIC CHEMISTRY
卷 56, 期 8, 页码 4576-4583出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.7b00149
关键词
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资金
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-ACO2-06CH11357]
- Knut and Alice Wallenberg Foundation
- Swedish Research Council (VR)
- Swedish Governmental Agency for Innovation Systems (VINNOVA) through the Berzelii Center EXSELENT on Porous Materials
- Beatriu de Pinos fellowship from Catalan Agency for Administration of University and Research [BP-DGR 2014]
- U.S. DOE Office of Science User Facility [DE-ACO2-06CH11357]
Here we describe the topological transformation of the pores of a new framework in the bio-MOF-100 family (dia-c) into the known isomer (Ics) by doubling the pore volume, which occurs during postsynthesis modifications. During this transformation, reassembling of the metal-organic framework (MOF) building blocks into a completely different framework occurs, involving breaking/forming of metal-ligand bonds. MOF crystallinity and local structure are retained, as determined by powder X-ray diffraction (PXRD) and pair distribution function (PDF) analyses, respectively. We exploited the inherent dynamism of bio-MOF-100 by coupling chemical decorations of the framework using solvent-assisted ligand exchange to the topological change. Following this method and starting from the pristine dense dia-c phase, open lcs-bio-MOF-100 was prepared and functionalized in situ with an iridium complex (IrL). Alternatively, the dia-c MOF could be modified with wide-ranging amounts of IrL up to ca. 50 mol %, as determined by solution H-1 NMR spectroscopy, by tuning the concentration of the solutions used and with no evidence for isomer transformation. The single-site nature of the iridium complexes within the MOFs was assessed by X-ray absorption spectroscopy (XAS) and PDF analyses. Ligand exchanges occurred quantitatively at room temperature, with no need of excess of the iridium metallolinker.
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