Low-entropy supramolecular crystals elucidating the inhomogeneity of interfacial water molecules at atomic resolution

Shinnosuke Horiuchi (), Shota Ogura, Kazuya Otsubo, Yuka Ikemoto, Hisao Kiuchi, Yudai Shinozaki, Hiromi Tsuyuki, Go Watanabe, Osamu Takahashi, Mikihiro Hayashi, Eri Sakuda, Yasuhiro Arikawa, Keisuke Umakoshi and Yoshihisa Harada
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Shinnosuke Horiuchi: The University of Tokyo
Shota Ogura: The University of Tokyo
Kazuya Otsubo: Tokyo University of Science
Yuka Ikemoto: Japan Synchrotron Radiation Research Institute
Hisao Kiuchi: The University of Tokyo
Yudai Shinozaki: Kitasato University
Hiromi Tsuyuki: Kitasato University
Go Watanabe: Kitasato University
Osamu Takahashi: Hiroshima University
Mikihiro Hayashi: Nagasaki University
Eri Sakuda: Nagasaki University
Yasuhiro Arikawa: Nagasaki University
Keisuke Umakoshi: Nagasaki University
Yoshihisa Harada: The University of Tokyo

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract Water at interfaces plays crucial roles in various natural phenomena and in the material sciences. Therefore, understanding the structure and hydrogen-bonding network at such interfaces is essential. Recent advances in porous crystalline materials, combined with single-crystal X-ray diffraction techniques, have enabled the visualization of molecular structures on pore surfaces at atomic resolution. Herein, we report the formation of a supramolecular porous crystal composed of a resorcin[4]arene and a rigid cationic coordination complex, stabilized by hydrogen bonds and noncovalent interactions. This specific arrangement creates a porous framework with anisotropic, information-rich surfaces, accommodating water molecules to form multi-layered water channels. The analysis reveals clustering motifs and hydrogen-bonding patterns in the water molecules at interfaces, supported by molecular dynamics simulations and spectroscopy studies. These findings advance our understanding of the structure–property relationship of water at interfaces in low-entropy crystalline materials, offering insights into their behavior on complex surfaces.

Date: 2025
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DOI: 10.1038/s41467-025-62578-0

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