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Ruoff, Rodney S.
Center for Multidimensional Carbon Materials (CMCM)
Research Interests
  • Next generation carbons, ultrathin sp3-bonded carbon sheets, negative curvature (‘Schwartzites’) carbons, sp3/sp2 hybrid carbon materials, model compounds for novel carbon materials, reaction mechanisms

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Partial Oxidation-Induced Electrical Conductivity and Paramagnetism in a Ni(II) Tetraaza[14]annulene-Linked Metal Organic Framework

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Title
Partial Oxidation-Induced Electrical Conductivity and Paramagnetism in a Ni(II) Tetraaza[14]annulene-Linked Metal Organic Framework
Author
Jiang, YiOh, InseonJoo, Se HunBuyukcakir, OnurChen, XiongLee, Sun HwaHuang, MingSeong, Won KyungKwak, Sang KyuYoo, Jung-WooRuoff, Rodney S.
Issue Date
2019-10
Publisher
American Chemical Society
Citation
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Abstract
We report the synthesis and characterization of a two-dimensional (2D) conjugated Ni(II) tetraaza[14]annulene-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).
URI
https://scholarworks.unist.ac.kr/handle/201301/27831
URL
https://pubs.acs.org/doi/10.1021/jacs.9b08601
DOI
10.1021/jacs.9b08601
ISSN
0002-7863
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