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Oriented Linear Self-Assembly of Colloidal Nanocrystals through Regioselective Formation of Hydrogen-Bonded Supramolecular Bridges
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    Oriented Linear Self-Assembly of Colloidal Nanocrystals through Regioselective Formation of Hydrogen-Bonded Supramolecular Bridges
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    • Siyu Wan
      Siyu Wan
      Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai 200433, China
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    • Yutong Gao
      Yutong Gao
      Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai 200433, China
      More by Yutong Gao
    • Zhebin Zhang
      Zhebin Zhang
      State Key Laboratory of Molecule Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai 200433, China
      More by Zhebin Zhang
    • Fangyue Wu
      Fangyue Wu
      Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai 200433, China
      More by Fangyue Wu
    • Ziyue Zheng
      Ziyue Zheng
      Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai 200433, China
      More by Ziyue Zheng
    • Hushui Chen
      Hushui Chen
      Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai 200433, China
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    • Xiangyun Xi
      Xiangyun Xi
      State Key Laboratory of Molecule Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai 200433, China
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    • Dong Yang
      Dong Yang
      State Key Laboratory of Molecule Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai 200433, China
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    • Tongtao Li*
      Tongtao Li
      Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai 200433, China
      *Email: [email protected]
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    • Zhihong Nie
      Zhihong Nie
      State Key Laboratory of Molecule Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai 200433, China
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    • Angang Dong*
      Angang Dong
      Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai 200433, China
      *Email: [email protected]
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    Other Access OptionsSupporting Information (1)

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 20, 14225–14234
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    https://doi.org/10.1021/jacs.4c03457
    Published May 8, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    The linear assembly of nanocrystals (NCs) with orientational order presents a significant challenge in the field of colloidal assembly. This study presents an efficient strategy for assembling oleic acid (OAH)-capped, faceted rare earth NCs─such as nanorods, nanoplates, and nanodumbbells─into flexible chain-like superstructures. Remarkably, these NC chains exhibit a high degree of particle orientation even with an interparticle distance reaching up to 15 nm. Central to this oriented assembly method is the facet-selective adsorption of low-molecular-weight polyethylene glycol (PEG), such as PEG-400 (Mn = 400), onto specific facets of NCs. This regioselectivity is achieved by exploiting the lower binding affinity of OAH ligands on the (100) facets of rare earth NCs, enabling facet-specific ligand displacement and subsequent PEG attachment. By adjusting the solvent polarity, the linear assembly of NCs is induced by the solvophobic effect, which simultaneously promotes the formation of hydrogen-bonded PEG supramolecular bridges. These supramolecular bridges effectively connect NCs and exhibit sufficient robustness to maintain the structural integrity of the chains, despite the large interparticle spacing. Notably, even when coassembling different types of NCs, the resulting multicomponent chains still feature highly selective facet-to-facet connections. This work not only introduces a versatile method for fabricating well-aligned linear superstructures but also provides valuable insights into the fundamental principles governing the facet-selective assembly of NCs in solution.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.4c03457.

    • Detailed synthesis and assembly of NC chains, additional TEM and optical images, histograms, DLS results, FTIR spectra, emission spectra, 1H NMR spectra, and TGA results (PDF)

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    This article is cited by 3 publications.

    1. Hong Tang, Takahiro Kojima, Kenji Kazumi, Kazuhiro Fukami, Hiroshi Sakaguchi. Surface-Modified Ruthenium Nanorods for an Ampere-Level Bifunctional Hydrogen Evolution Reaction/Oxygen Evolution Reaction Electrocatalyst. ACS Applied Materials & Interfaces 2024, 16 (27) , 35053-35062. https://doi.org/10.1021/acsami.4c05286
    2. Xiaojun Ding, Qiang Gao, Yi Su, Jing Chen, Gang Ye. Pi‐Stacking Geometry Directed Supramolecular Secondary Building Units Shaping Hydrogen‐Bonded Frameworks for Intensive NH 3 Adsorption. Angewandte Chemie International Edition 2025, 36 https://doi.org/10.1002/anie.202500268
    3. Xiaojun Ding, Qiang Gao, Yi Su, Jing Chen, Gang Ye. Pi‐Stacking Geometry Directed Supramolecular Secondary Building Units Shaping Hydrogen‐Bonded Frameworks for Intensive NH 3 Adsorption. Angewandte Chemie 2025, 36 https://doi.org/10.1002/ange.202500268

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 20, 14225–14234
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.4c03457
    Published May 8, 2024
    Copyright © 2024 American Chemical Society

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