Synthesizing Interpenetrated Triazine‐based Covalent Organic Frameworks from CO2

Author:

Zhang Siquan1ORCID,Lombardo Loris2ORCID,Tsujimoto Masahiko2,Fan Zeyu1,Berdichevsky Ellan K.1ORCID,Wei Yong‐Sheng2,Kageyama Kotoha1,Nishiyama Yusuke3,Horike Satoshi245ORCID

Affiliation:

1. Department of Synthetic Chemistry and Biological Chemistry Graduate School of Engineering Kyoto University, Katsura, Nishikyo-ku Kyoto 615-8510 Japan

2. Institute for Integrated Cell-Material Sciences Institute for Advanced Study Kyoto University, Yoshida-Honmachi, Sakyo-ku Kyoto 606-8501 Japan

3. JEOL Ltd. Akishima Tokyo 196-8558 Japan

4. Department of Materials Science and Engineering School of Molecular Science and Engineering Vidyasirimedhi Institute of Science and Technology Rayong 21210 Thailand

5. Department of Chemistry Graduate School of Science Kyoto University, Kitashirakawa-Oiwakecho, Sakyo-ku Kyoto 606-8502 Japan

Abstract

AbstractCrystalline triazine‐based covalent organic frameworks (COFs) are aromatic nitrogen‐rich porous materials. COFs typically show high thermal/chemical stability, and are promising for energy applications, but often require harsh synthesis conditions and suffer from low crystallinity. In this work, we propose an environmentally friendly route for the synthesis of crystalline COFs from CO2 molecules as a precursor. The mass ratio of CO2 conversion into COFs formula unit reaches 46.3 %. The synthesis consists of two steps; preparation of 1,4‐piperazinedicarboxaldehyde from CO2 and piperazine, and condensation of the dicarboxaldehyde and melamine to construct the framework. The CO2‐derived COF has a 3‐fold interpenetrated structure of 2D layers determined by powder X‐ray diffraction, high‐resolution transmission electron microscopy, and select‐area electron diffraction. The structure shows a high Brunauer–Emmett–Teller surface area of 945 m2 g−1 and high stability against strong acid (6 M HCl), base (6 M NaOH), and boiling water over 24 hours. Post‐modification of the framework with oxone has been demonstrated to modulate hydrophilicity, and it exhibits proton conductivity of 2.5×10−2 S cm−1 at 85 °C, 95 % of relative humidity.

Funder

China Scholarship Council

Japan Society for the Promotion of Science

Publisher

Wiley

Subject

General Medicine

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