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Synthesis of ordered carbonaceous frameworks from organic crystals

Author

Listed:
  • Hirotomo Nishihara

    (Tohoku University
    PRESTO, the Japan Science and Technology Agency (JST))

  • Tetsuya Hirota

    (Tohoku University)

  • Kenta Matsuura

    (Tohoku University)

  • Mao Ohwada

    (Tohoku University)

  • Norihisa Hoshino

    (Tohoku University)

  • Tomoyuki Akutagawa

    (Tohoku University)

  • Takeshi Higuchi

    (Tohoku University)

  • Hiroshi Jinnai

    (Tohoku University)

  • Yoshitaka Koseki

    (Tohoku University)

  • Hitoshi Kasai

    (Tohoku University)

  • Yoshiaki Matsuo

    (University of Hyogo)

  • Jun Maruyama

    (Osaka Research Institute of Industrial Science and Technology)

  • Yuichiro Hayasaka

    (Tohoku University)

  • Hisashi Konaka

    (X-ray Instrument Divistion, Rigaku Corporation)

  • Yasuhiro Yamada

    (Chiba University)

  • Shingi Yamaguchi

    (The University of Tokyo)

  • Kazuhide Kamiya

    (PRESTO, the Japan Science and Technology Agency (JST)
    Osaka University)

  • Takuya Kamimura

    (Kyushu University)

  • Hirofumi Nobukuni

    (Kyushu University)

  • Fumito Tani

    (Kyushu University)

Abstract

Despite recent advances in the carbonization of organic crystalline solids like metal-organic frameworks or supramolecular frameworks, it has been challenging to convert crystalline organic solids into ordered carbonaceous frameworks. Herein, we report a route to attaining such ordered frameworks via the carbonization of an organic crystal of a Ni-containing cyclic porphyrin dimer (Ni2-CPDPy). This dimer comprises two Ni–porphyrins linked by two butadiyne (diacetylene) moieties through phenyl groups. The Ni2-CPDPy crystal is thermally converted into a crystalline covalent-organic framework at 581 K and is further converted into ordered carbonaceous frameworks equipped with electrical conductivity by subsequent carbonization at 873–1073 K. In addition, the porphyrin’s Ni–N4 unit is also well retained and embedded in the final framework. The resulting ordered carbonaceous frameworks exhibit an intermediate structure, between organic-based frameworks and carbon materials, with advantageous electrocatalysis. This principle enables the chemical molecular-level structural design of three-dimensional carbonaceous frameworks.

Suggested Citation

  • Hirotomo Nishihara & Tetsuya Hirota & Kenta Matsuura & Mao Ohwada & Norihisa Hoshino & Tomoyuki Akutagawa & Takeshi Higuchi & Hiroshi Jinnai & Yoshitaka Koseki & Hitoshi Kasai & Yoshiaki Matsuo & Jun , 2017. "Synthesis of ordered carbonaceous frameworks from organic crystals," Nature Communications, Nature, vol. 8(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_s41467-017-00152-z
    DOI: 10.1038/s41467-017-00152-z
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