Metal-hydrogen-pi-bonded organic frameworks

Zhu, Jie; Samperisi, Laura; Kalaj, Mark; Chiong, Jerika A.; Bailey, Jake B.; Zhang, Zhiyin; Yu, Chung-Jui; Sikma, R. Eric; Zou, Xiaodong; Cohen, Seth M.; Huang, Zhehao; Tezcan, F. Akif

doi:10.1039/d1dt04278e

Title: Metal-hydrogen-pi-bonded organic frameworks

Journal Article · 04 January 2022 · Dalton Transactions

DOI: https://doi.org/10.1039/d1dt04278e · OSTI ID:1871937

Zhu, Jie ^[1]; Samperisi, Laura ^[2];

^[3];

^[3]; Bailey, Jake B. ^[3]; Zhang, Zhiyin ^[3]; Yu, Chung-Jui ^[3]; Sikma, R. Eric ^[3];

^[2];

^[2]

Univ. of California, San Diego, La Jolla, CA (United States); U.C. San Diego
Stockholm Univ. (Sweden)
Univ. of California, San Diego, La Jolla, CA (United States)

We report the synthesis and characterization of a new series of permanently porous, three-dimensional metal–organic frameworks (MOFs), M-HAF-2 (M = Fe, Ga, or In), constructed from tetratopic, hydroxamate-based, chelating linkers. Here, the structure of M-HAF-2 was determined by three-dimensional electron diffraction (3D ED), revealing a unique interpenetrated hcb-a net topology. This unusual topology is enabled by the presence of free hydroxamic acid groups, which lead to the formation of a diverse network of cooperative interactions comprising metal–hydroxamate coordination interactions at single metal nodes, staggered π–π interactions between linkers, and H-bonding interactions between metal-coordinated and free hydroxamate groups. Such extensive, multimodal interconnectivity is reminiscent of the complex, noncovalent interaction networks of proteins and endows M-HAF-2 frameworks with high thermal and chemical stability and allows them to readily undergo postsynthetic metal ion exchange (PSE) between trivalent metal ions. We demonstrate that M-HAF-2 can serve as versatile porous materials for ionic separations, aided by one-dimensional channels lined by continuously π-stacked aromatic groups and H-bonding hydroxamate functionalities. As an addition to the small group of hydroxamic acid-based MOFs, M-HAF-2 represents a structural merger between MOFs and hydrogen-bonded organic frameworks (HOFs) and illustrates the utility of non-canonical metal-coordinating functionalities in the discovery of new bonding and topological patterns in reticular materials.

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Research Organization:: Univ. of California, San Diego, La Jolla, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; Swedish Research Council Formas; Knut and Alice Wallenberg Foundation

Grant/Contract Number:: FG02-08ER46519

OSTI ID:: 1871937

Journal Information:: Dalton Transactions, Journal Name: Dalton Transactions Journal Issue: 5 Vol. 51; ISSN 1477-9226

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
MOFs
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Title: Metal-hydrogen-pi-bonded organic frameworks

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