Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 46, Pages 16682-16690Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201910717
Keywords
heterogeneous catalysis; linker desymmetrization; metal-organic frameworks; structural evolution; topology
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Funding
- National Natural Science Foundation of China (NSFC) [21875285, 21571187]
- Taishan Scholar Foundation [ts201511019]
- Center for Gas Separations, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0001015]
- Robert A. Welch Foundation through a Welch Endowed Chair [A-0030]
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Linker desymmetrization has been witnessed as a powerful design strategy for the discovery of highly connected metal-organic frameworks (MOFs) with unprecedented topologies. Herein, we introduce molecular pivot-hinge installation as a linker desymmetrization strategy to evolve the topology of highly connected rare-earth (RE) MOFs, where a pivot group is placed in the center of a linker similar to a hinge. By tuning the composition of pivot groups and steric hindrances of the substituents on various linker rotamers, MOFs with various topologies can be obtained. The combination of L-SO2 with C-2v symmetry and 12-connected RE9 clusters leads to the formation of a fascinating (4,12)-c dfs new topology. Interestingly, when replacing L-SO2 with a tetrahedra linker L-O, the stacking behaviors of RE-organic layers switch from an eclipsed mode to a staggered stacking mode, leading to the discovery of an intriguing hjz topology. Additionally, the combination of the RE cluster and a linker [(L-(CH3)(6))] with more bulky groups gives rise to a flu topology with a new 8-c inorganic cluster. The diversity of these RE-MOFs was further enhanced through post-synthetic installation of linkers with various functional groups. Functionalization of each linker with acidic and basic units in the mesoporous RE-based PCN-905-SO2 allows for efficient cascade catalytic transformation within the functionalized channels.
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