Low-entropy supramolecular crystals elucidating the inhomogeneity of interfacial water molecules at atomic resolution
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.
Authors
- Mikihiro Hayashi (ORCID: https://orcid.org/0000-0002-1386-847X)
- Kazuya Otsubo (ORCID: https://orcid.org/0000-0003-4688-2822)
- Shinnosuke Horiuchi (ORCID: https://orcid.org/0000-0002-5692-6377)
- Eri Sakuda (ORCID: https://orcid.org/0000-0001-9882-7628)
- Yuka Ikemoto
- Keisuke Umakoshi (ORCID: https://orcid.org/0000-0002-2027-6333)
- Yoshihisa Harada (ORCID: https://orcid.org/0000-0002-4590-9109)
- Yasuhiro Arikawa (ORCID: https://orcid.org/0000-0001-6727-2340)
- Hiromi Tsuyuki
- Go Watanabe (ORCID: https://orcid.org/0000-0001-6713-1249)
- Hisao Kiuchi (ORCID: https://orcid.org/0000-0001-9139-8218)
- Shohei Ogura (ORCID: https://orcid.org/0000-0002-8580-5021)
- Osamu Takahashi (ORCID: https://orcid.org/0000-0002-5321-1747)
- Yudai Shinozaki
Institutions
- Hiroshima University (JP)
- University of Nagasaki (JP)
- Tokyo University of Science (JP)
- Tokyo University of the Arts (JP)
- Japan Synchrotron Radiation Research Institute (JP)
- Nagasaki University (JP)
- Kitasato University (JP)
- The University of Tokyo (JP)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-08-29
- DOI
- https://doi.org/10.1038/s41467-025-62578-0
- Citations
- 1
- Primary Topic
- nanoparticles nucleation surface interactions
- Type
- article
- Field-Weighted Citation Impact
- 1.30
Funders
- Kurita Water and Environment Foundation
- Ministry of Education, Culture, Sports, Science and Technology
- University of Tokyo
- SEI Group CSR Foundation
- Japan Society for the Promotion of Science
- Research Institute for Information Technology, Kyushu University