Roles of Alkali Metals and Ionic Networks in Directing the Formation of Anionic Metal–Organic Frameworks

Hong, Anh N.; Yang, Huajun; Zhou, Angel; Bu, Xianhui; Feng, Pingyun

doi:10.1021/acs.cgd.0c00827

Title: Roles of Alkali Metals and Ionic Networks in Directing the Formation of Anionic Metal–Organic Frameworks

Journal Article · Fri Sep 11 00:00:00 EDT 2020 · Crystal Growth and Design

DOI:https://doi.org/10.1021/acs.cgd.0c00827· OSTI ID:1755104

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^[2]; Zhou, Angel ^[1];

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Univ. of California, Riverside, CA (United States)
California State Univ. (CalState), Long Beach, CA (United States)

Integrating different types of fundamental chemical interactions to direct the self-assembly processes and to control the dimension of the network formed by each type of interactions is a promising strategy to develop advanced functional materials. Here, the ionic interaction of alkali metals (Na, K, Cs) towards multi-functional 2,2’-disulfo-4,4’-oxydibenzoic acid is utilized in two solvent systems, aqueous-amide and uro-amide, to synthesize six novel anionic framework materials with dramatically different features and dimensionalities: (Na₃[Zn₄O(L^4-)₃(e-murea)(H₂O)₃](H₂N(CH₃)₂+)₃ (CPM-s1), [Zn₄O(L^4-)₃(DMF)]((NH₂(CH₃)₂+)₆) (CPM-s2), Na₆[(Zn₂OH₂)₃(L^3-)₆](H₂O)₃ (CPM-s3), K₃[Zn₂(L^4-)₂](H₂N(CH₃)₂+)(e-murea)₂(H₂O)₃ (CPM-s4), K₄[Zn(L^3-)₂](H₂O)₂ (CPM-s5), and Cs₆[Zn(L^4-)₂](H₂O)₂ (CPM-s6), L^4- = 2,2’-disulfo-4,4’-oxydibenzoate, DMF = N,N-dimethylformamide, e-murea = 1,3-dimethyl-1-2-imidazolidinone). In CPM-s1 to CPM-s6, the alkali-sulfonate ionic bonding networks transformed from 0D clusters with Na⁺ to 1D chains and 2D sheets with K⁺, and 3D network with Cs⁺. These vastly differing ionic domains influenced the coordination modes and spatial arrangements of the metal-carboxylate linkers, which consequently, directed the dimensionality of the coordination networks from 3D with Na⁺ to 1D with Cs⁺. CPM-s1 and CPM-s2, made from tetrameric Zn₄O clusters are rare examples of anionic MOF-5-type structures. CPM-s3 features an unprecedented hexameric Zn₆ cluster. Even though a large portion of the charge-balancing cations in these materials would hamper hydrogen bonding networks, some of them still exhibit very high ionic conductivity (e.g. 1.25 x 10^-3 S cm^-1 in CPM-s3), suggesting the potential of these materials as solid-state electrolytes.

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Research Organization:: Univ. of California, Riverside, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0010596

OSTI ID:: 1755104

Journal Information:: Crystal Growth and Design, Vol. 20, Issue 10; ISSN 1528-7483

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Roles of Alkali Metals and Ionic Networks in Directing the Formation of Anionic Metal–Organic Frameworks

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