Partial Oxidation-Induced Electrical Conductivity and Paramagnetism in a Ni(II) Tetraazaannulene-Linked Metal Organic Framework
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- Partial Oxidation-Induced Electrical Conductivity and Paramagnetism in a Ni(II) Tetraazaannulene-Linked Metal Organic Framework
- Jiang, Yi; Oh, Inseon; Joo, Se Hun; Buyukcakir, Onur; Chen, Xiong; Lee, Sun Hwa; Huang, Ming; Seong, Won Kyung; Kwak, Sang Kyu; Yoo, Jung-Woo; Ruoff, Rodney S.
- Issue Date
- American Chemical Society
- JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.141, no.42, pp.16884 - 16893
- We report the synthesis and characterization of a two-dimensional (2D) conjugated Ni(II) tetraazaannulene-linked metal organic framework (NiTAA-MOF) where NiTAA is a macrocyclic MN4 (M = metal, N = nitrogen) compound. The structure of NiTAA-MOF was elucidated by Fourier-transform infrared, X-ray photoemission, and X-ray diffraction spectroscopies, in combination with density functional theory (DFT) calculations. When chemically oxidized by iodine, the insulating bulk NiTAA-MOF (σ < 10–10 S/cm) exhibits an electrical conductivity of 0.01 S/cm at 300 K, demonstrating the vital role of ligand oxidation in the electrical conductivity of 2D MOFs. Magnetization measurements show that iodine-doped NiTAA-MOF is paramagnetic with weak antiferromagnetic coupling due to the presence of organic radicals of oxidized ligands and high-spin Ni(II) sites of the missing-linker defects. In addition to providing further insights into the origin of the induced electrical conductivity in 2D MOFs, both pristine and iodine-doped NiTAA-MOF synthesized in this work could find potential applications in areas such as catalase mimics, catalysis, energy storage, and dynamic nuclear polarization-nuclear magnetic resonance (DNP-NMR).
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