Creating Hierarchical Pores by Controlled Linker Thermolysis in Multivariate Metal–Organic Frameworks

Feng, Liang; Yuan, Shuai; Zhang, Liang-Liang; Tan, Kui; Li, Jia-Luo; Kirchon, Angelo; Liu, Ling-Mei; Zhang, Peng; Han, Yu; Chabal, Yves J.; Zhou, Hong-Cai

doi:10.1021/jacs.7b12916

Creating Hierarchical Pores by Controlled Linker Thermolysis in Multivariate Metal–Organic Frameworks

Journal Article · Thu Jan 18 00:00:00 EST 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b12916· OSTI ID:1470336

^[1]; Yuan, Shuai ^[1]; Zhang, Liang-Liang ^[1]; ^[2]; Li, Jia-Luo ^[1]; Kirchon, Angelo ^[1]; Liu, Ling-Mei ^[3]; Zhang, Peng ^[1]; ^[3]; ^[2]; ^[1]

Texas A & M Univ., College Station, TX (United States)
Univ. of Texas at Dallas, Richardson, TX (United States)
King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia)

Sufficient pore size, appropriate stability, and hierarchical porosity are three prerequisites for open frameworks designed for drug delivery, enzyme immobilization, and catalysis involving large molecules. In this work, we report a powerful and general strategy, linker thermolysis, to construct ultrastable hierarchically porous metal–organic frameworks (HP-MOFs) with tunable pore size distribution. Linker instability, usually an undesirable trait of MOFs, was exploited to create mesopores by generating crystal defects throughout a microporous MOF crystal via thermolysis. The crystallinity and stability of HP-MOFs remain after thermolabile linkers are selectively removed from multivariate metal–organic frameworks (MTV-MOFs) through a decarboxylation process. A domain-based linker spatial distribution was found to be critical for creating hierarchical pores inside MTV-MOFs. Furthermore, linker thermolysis promotes the formation of ultrasmall metal oxide nanoparticles immobilized in an open framework that exhibits high catalytic activity for Lewis acid-catalyzed reactions. Lastly and most importantly, this work provides fresh insights into the connection between linker apportionment and vacancy distribution, which may shed light on probing the disordered linker apportionment in multivariate systems, a long-standing challenge in the study of MTV-MOFs.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: FE0026472; FG02-08ER46491; SC0001015

OSTI ID:: 1470336

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 6 Vol. 140; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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