Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 26, Pages 14601-14608Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202103104
Keywords
hierarchically porous MOFs; mesopore engineering; molecular surgery; molecules encapsulation; plane-oriented etching
Categories
Funding
- Hefei National Laboratory for Physical Sciences at the Microscale
- Hefei Science Center of Chinese Academy of Sciences
- National Synchrotron Radiation Laboratory
- Fujian Institute of Innovation of Chinese Academy of Sciences
- National Natural Science Foundation of China (NSFC) [21571167, 51502282, 22075266]
- Fundamental Research Funds for the Central Universities [WK2060190053, WK2060190100]
- Anhui Province Natural Science Foundation [1608085MB28]
- CAS-TWAS President's PhD fellowship
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Hierarchically porous MOFs (HP-MOFs) exhibit advantageous synergism of micro- and mesopore structures, but face challenges in synthetic control at a molecular scale. This study presents a novel approach for reversible and controllable mesopore generation and renovation in microporous MOFs like HKUST-1, achieved through gas-phase etching to create uniform mesopores without altering crystal size or morphology. The generated mesopores can be further modified using MOF precursor solutions, demonstrating a powerful protocol for precisely tailoring and tuning the properties of MOF materials at a molecular scale.
Hierarchically porous MOFs (HP-MOFs) present advantageous synergism of micro- and mesopore but challenging in synthetic control at molecular scale. Herein, we present the first example of reversible and controllable mesopore generation and renovation in a microporous MOF of HKUST-1 via synthetic manipulation at molecular scale. An ammonia-gas etching strategy is proposed to create mesopores in carboxylate-based microporous MOFs and thus produce HP-MOFs. Gas-phase etching ensures uniform mesopore formation inside the MOF crystals via plane-oriented cutting the carboxylate-metal bonds off without affecting the crystal size and morphology. The mesopore size is controlled by the etching temperature, while the mesopore volume could be tuned by adjusting etchant pressure. The generated mesopores could be renovated using MOF precursors solutions so that to achieve controllable mesopore generation/closure, and encapsulation of the adsorbed molecules. This work demonstrates a powerful protocol for precisely tailoring and tuning the properties of MOF materials at molecular scale.
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