Synthesis, structure and photocatalysis properties of two 3D Isostructural Ln (III)-MOFs based 2,6-Pyridinedicarboxylic acid

doi:10.1016/j.jmst.2018.03.011

Abstract

Abstract:

Two new 3D metal-organic frameworks (MOFs) named [Pr₂(PDA)₃·3H₂O]·H₂O (1) and [Nd₂(PDA)₃·3H₂O]·H₂O (2) [2,6-Pyridinedicarboxylic acid (H₂PDA)] were synthesized by solvothermal method. They were characterized by elemental analyses (EA), infrared spectroscopy (FT-IR), thermogravimetric analysis (TG), photocatalysis performance and single crystal X-ray diffraction studies (XRD). The XRD analysis indicated that MOFs (1) and (2) both belong to the monoclinic system with space group P2(1)/C. The structural model were drawn by the diamond software, and the structure revel that MOFs (1) and (2) adopt three-dimensional (3D) frameworks constructed by cross-linking of one-dimensional (1D) infinite chain secondary building unit (SBU) by 2,6-Pyridinedicarboxylic acid and hydrogen bond as linker. These frameworks feature channels inside which coordinated H₂O solvent molecules are located. Thermogravimetric analysis showed that both MOFs are thermally stable, the photocatalytic evaluation showed the materials have a good prospect in degration methylene blue. As for complex 1, the decomposition efficiency of Methylene blue was about 91.08% after 130 min and the complex 2 reach 90.45% after 160 min under the sun light.

Key words: Metal-organic frameworks, Solvothermal method, Photocatalysis performance

Chenchen Zhang, Siyue Wei, Lixian Sun, Fen Xu, Pengru Huang, Hongliang Peng. Synthesis, structure and photocatalysis properties of two 3D Isostructural Ln (III)-MOFs based 2,6-Pyridinedicarboxylic acid[J]. J. Mater. Sci. Technol., 2018, 34(9): 1526-1531.

Figures/Tables 7

Table 1 Crystallographic Details of complexes 1-2.

Chemical formula	C₂₁H₁₉N₃O₁₆Pr₂	C₂₁H₁₉N₃O₁₆Nd₂
Formula mass	851.21	857.87
Crystal system	monoclinic	monoclinic
a (?)	10.9850(7)	10.9754(11)
b (?)	17.5385(12)	17.4982(17)
c (?)	13.4684(9)	13.4142(14)
β (deg)	101.041(2)	101.175(4)
Unit cell vol (?³)	2546.8(3)	2527.3(4)
Space group	P2(1)/C	P2(1)/C
Z	4	4
Radiation type	Mo Kα	Mo Kα
Absorption coefficient	3.896	4.152
Reflections collected	25830/6273	23246/6203
Limiting indices	12 < = h < = 14; -21 < = k < = 23 - 17 < = l < = 17	-13 < = h < = 14; -23 < = k < = 23 - 17 < = l < = 17
F (000)	1648.0	1656.0
Rint	0.0312	0.0393
Fina R indices (I > 2σ(I))	R1 = 0.0225, Wr2 = 0.0573	R1 = 0.0412, Wr2 = 0.1088
R indices (all data)	R1 = 0.0252, Wr2 = 0.0587	R1 = 0.0522, Wr2 = 0.1222
GOF on F²	1.104	1.184

Table 2 Selected bond lengths (nm) bond angles (°) for 1-2.

Fig. 1. (a) Coordination environment of PrIII atom in 1 (Symmetry codes: (#1) 2-x, 1-y, 1-z; (#2) -1 + x, y, z; (#3) x, 0.5-y, 0.5 + z; (#4) 1-x, 1-y, 1-z), (b) One-dimensional chain structure of complex 1, (c) The 2D structure of complex1, (d) The 3D supramolecular net.

Fig. 2. (a) Coordination environment of NdIII atom in 2 (Symmetry codes: (#1) x-1, y, z; (#2) 2-x, 1-y, 1-z; (#3) 1-x, 1-y, 1-z; (#4) x, 0.5-y, 0.5 + z), (b) One-dimensional chain structure of complex 2, (c) 2D structure of complex 2, (d) 3D supramolecular net.

Fig. 3. (a) IR spectra for ligand and two complexes, (b) The thermogravimetric analysis of two complexes.

Fig. 4. Powder X-ray diffraction spectra of simulated and synthesized complexes 1 and 2.

Fig. 5. (a) Photocatalytic performance of complex 1, (b) Degradation efficiency of complex 1, (c) Photocatalytic performance of complex 2, (d) Degradation efficiency of complex 2.

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