Precise Control of the Dimension of Homochiral Metal-Organic Frameworks （MOFs) and Their Luminescence Properties

doi:10.6023/A21100474

Abstract

To precisely control the construction of different dimensional and topological structure represents one of the most challenging issues facing synthetic chemistry nowadays, especially synthesizing different dimensions of chiral materials with identical compositions. Self-assembly of structural dimension of hybrid materials based on coordination chemistry has been regarded as an effective means addressed this issue. Herein, self-assembly of Zn salts with R,R-CHCAIP (5,5′-((1R,2R)-cyclohexane dicarbonyl bis(azanediyl)) diisophthalic acid) generates a new 3D homochiral metal-organic framework Zn_1.5(R,R-CHCAIP)(H₂O)₂ (HMOF-4) that uses the same ligand and metal as our reported 1D tube Zn₂(R,R-CHCAIP)Py₂(H₂O) (HMOF-2) and 2D layer [Zn₄(R,R-CHCAIP)₂(4,4′-bipy)₂(H₂O)₅]•5H₂O•3DMA (HMOF-3, DMA, N,N-dimethylacetamide) under the solvothermal reaction at high temperature (100 ℃). Based on a new strategy of the synergistic action of the auxiliary ligand and temperature, the structural diversity for HMOF-2, HMOF-3 and HMOF-4 from 1D to 2D and 3D is modulated during the assembly process, and the resulting multidimensional homochiral MOFs with identical composition are extremely rare in currently reported MOFs with different dimensions. The fluorescence of HMOF-4 and HMOF-2, HMOF-3 is investigated, and their fluorescent mechanisms are interpreted by time-dependent density functional theory (TDDFT) calculation. The tiny difference of their fluorescent emission spectra indicates the dimensions of Zn-MOFs have little effect on fluorescence. This work provides a distinctive construction means for precise control of the different dimension of homochiral MOFs.

Key words: precise control, homochiral metal-organic frameworks (MOFs), dimension, synergistic action, fluorescence

Cite this article

Yan-Wu Zhao, Xing Li, Fu-Qiang Zhang, Xiang Zhang. Precise Control of the Dimension of Homochiral Metal-Organic Frameworks （MOFs) and Their Luminescence Properties[J]. Acta Chimica Sinica, 2021, 79(11): 1409-1414.

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Fig. & Tab. 7

Figure 1. The construction of homochiral 1D metal-organic nanotube (HMOF-2), 2D wave-like layer (HMOF-3) and 3D framework of HMOF-4

Figure 2. (a) Representation of Zn coordination environment in HMOF-4. Symmetry operation: a: 1–y, 1–x, 1/2–z; b: 1/2+x, 1/2–y, 3/4–z; c: –1/2+x, 3/2–y, 3/4–z; (b) topological type: flu (sqc169), (4,8)-connected net in HMOF-4 (bright green: Zn2(COO)4(H2O)2 SBUs, bluish violet: R,R-CHCAIP ligand); (c) coordination mode of organic ligand R,R-CHCAIP in HMOF-4; (d) and (e) trinuclear cluster with the coordination around Zn1 and Zn2, showing octahedral and tetrahedral geometries, respectively

Figure 3. XPS spectra of HMOF-4: (a) survey spectra, (b) Zn 2p, (c) C 1s, (d) O 1s and (e) N 1s

Figure 4. IR spectra of the organic ligand (violet line) and HMOF-4 (black line)

Figure 5. TGA curve of HMOF-4

Figure 6. (a) Excitation and emission spectra of solid HMOF-4; (b) emission spectra of solid R,R-CHCAIP ligand, HMOF-2, HMOF-3 and HMOF-4

Figure 7. Energy-level diagram depicting the dominant transitions that comprise the lowest-energy absorption bands for (a) organic ligand, (b) HMOF-2 and (c) HMOF-3

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