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Modulating vectored non-covalent interactions for layered assembly with engineerable properties

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Abstract

Vectored non-covalent interactions—mainly hydrogen bonding and aromatic interactions—extensively contribute to (bio)-organic self-assembling processes and significantly impact the physicochemical properties of the associated superstructures. However, vectored non-covalent interaction-driven assembly occurs mainly along one-dimensional (1D) or three-dimensional (3D) directions, and a two-dimensional (2D) orientation, especially that of multilayered, graphene-like assembly, has been reported less. In this present research, by introducing amino, hydroxyl, and phenyl moieties to the triazine skeleton, supramolecular layered assembly is achieved by vectored non-covalent interactions. The planar hydrogen bonding network results in high stability, with a thermal sustainability of up to about 330 °C and a Young’s modulus of up to about 40 GPa. Upon introducing wrinkles by biased hydrogen bonding or aromatic interactions to disturb the planar organization, the stability attenuates. However, the intertwined aromatic interactions prompt a red edge excitation shift effect inside the assemblies, inducing broad-spectrum fluorescence covering nearly the entire visible light region (400–650 nm). We show that bionic, superhydrophobic, pillar-like arrays with contact angles of up to about 170° can be engineered by aromatic interactions using a physical vapor deposition approach, which cannot be realized through hydrogen bonding. Our findings show the feasibility of 2D assembly with engineerable properties by modulating vectored non-covalent interactions.

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Acknowledgements

This work was supported by the Fund for Creative Research Groups of National Natural Science Foundation of China (No. 51821093), the National Natural Science Foundation of China (Nos. 52175551, 52075484) (KT and DM), the National Key Research and Development Program (SQ2021YFE010405) (KT) and Science Foundation Ireland (SFI) through awards Nos. 15/CDA/3491 and 12/RC/2275_P2 (DT), and computing resources at the SFI/Higher Education Authority Irish Center for High-End Computing (ICHEC) (SG and DT). The authors thank Dr. Sigal Rencus-Lazar for language editing and the members of all the laboratories for helpful discussions.

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  1. Jiahao Zhang and Sarah Guerin have contributed equally to this work.

Authors and Affiliations

  1. State Key Laboratory of Fluid Power and Mechatronic Systems, School of Mechanical Engineering, Zhejiang University, Hangzhou, 310027, China

    Jiahao Zhang, Haoran Wu, Yancheng Wang, Kai Tao & Deqing Mei

  2. Future Science Research Institute, Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou, 311200, China

    Jiahao Zhang, Haoran Wu & Kai Tao

  3. Department of Physics and Bernal Institute, University of Limerick, Castletroy, Co. Limerick, Limerick, V94T9PX, Ireland

    Sarah Guerin, Syed A. M. Tofail & Damien Thompson

  4. National Laboratory of Solid State Microstructure, Department of Physics, Nanjing University, Nanjing, 210093, China

    Bin Xue, Yi Cao & Wei Wang

  5. Key Laboratory of Advanced Manufacturing Technology of Zhejiang Province, School of Mechanical Engineering, Zhejiang University, Hangzhou, 310027, China

    Yancheng Wang, Kai Tao & Deqing Mei

  6. School of Molecular Cell Biology and Biotechnology, George S. Wise Faculty of Life Sciences, Tel Aviv University, 6997801, Tel Aviv, Israel

    Ehud Gazit

  7. Department of Materials Science and Engineering, Iby and Aladar Fleischman Faculty of Engineering, Tel Aviv University, 6997801, Tel Aviv, Israel

    Ehud Gazit

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  1. Jiahao Zhang
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  2. Sarah Guerin
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  3. Haoran Wu
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  4. Bin Xue
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  9. Wei Wang
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  10. Kai Tao
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  11. Deqing Mei
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Contributions

All authors contributed to this manuscript and gave permission for the final version of the publication. BX, DT, and KT conceived and designed the work; JZ, HW, YW, and DM conducted the crystal growth and further characterizations; BX, YC, and WW conducted the Young’s model measurement; JZ, HW, and EG performed the TGA experiments; JZ, HW, YW, DM, and EG fabricated the PVD system and the coating film; SG, SAMT, and DT carried out theoretical calculations; JZ and SG coordinated all the work, analyzed the results, wrote and edited the manuscript with input from all authors.

Corresponding authors

Correspondence to Bin Xue, Damien Thompson or Kai Tao.

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This study does not contain any studies with human or animal subjects performed by any of the authors.

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Zhang, J., Guerin, S., Wu, H. et al. Modulating vectored non-covalent interactions for layered assembly with engineerable properties. Bio-des. Manuf. 5, 529–539 (2022). https://doi.org/10.1007/s42242-022-00186-3

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  • DOI: https://doi.org/10.1007/s42242-022-00186-3

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