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Molecular basis of cooperativity in pH-triggered supramolecular self-assembly

Author

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  • Yang Li

    (Simmons Comprehensive Cancer Center, University of Texas Southwestern Medical Center)

  • Tian Zhao

    (Simmons Comprehensive Cancer Center, University of Texas Southwestern Medical Center)

  • Chensu Wang

    (Simmons Comprehensive Cancer Center, University of Texas Southwestern Medical Center
    University of Texas Southwestern Medical Center)

  • Zhiqiang Lin

    (Simmons Comprehensive Cancer Center, University of Texas Southwestern Medical Center)

  • Gang Huang

    (Simmons Comprehensive Cancer Center, University of Texas Southwestern Medical Center)

  • Baran D. Sumer

    (University of Texas Southwestern Medical Center)

  • Jinming Gao

    (Simmons Comprehensive Cancer Center, University of Texas Southwestern Medical Center)

Abstract

Supramolecular self-assembly offers a powerful strategy to produce high-performance, stimuli-responsive nanomaterials. However, lack of molecular understanding of stimulated responses frequently hampers our ability to rationally design nanomaterials with sharp responses. Here we elucidated the molecular pathway of pH-triggered supramolecular self-assembly of a series of ultra-pH sensitive (UPS) block copolymers. Hydrophobic micellization drove divergent proton distribution in either highly protonated unimer or neutral micelle states along the majority of the titration coordinate unlike conventional small molecular or polymeric bases. This all-or-nothing two-state solution is a hallmark of positive cooperativity. Integrated modelling and experimental validation yielded a Hill coefficient of 51 in pH cooperativity for a representative UPS block copolymer, by far the largest reported in the literature. These data suggest hydrophobic micellization and resulting positive cooperativity offer a versatile strategy to convert responsive nanomaterials into binary on/off switchable systems for chemical and biological sensing, as demonstrated in an additional anion sensing model.

Suggested Citation

  • Yang Li & Tian Zhao & Chensu Wang & Zhiqiang Lin & Gang Huang & Baran D. Sumer & Jinming Gao, 2016. "Molecular basis of cooperativity in pH-triggered supramolecular self-assembly," Nature Communications, Nature, vol. 7(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13214
    DOI: 10.1038/ncomms13214
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    Cited by:

    1. Jian Cheng & Guihai Gan & Shaoqiu Zheng & Guoying Zhang & Chen Zhu & Shiyong Liu & Jinming Hu, 2023. "Biofilm heterogeneity-adaptive photoredox catalysis enables red light-triggered nitric oxide release for combating drug-resistant infections," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Yue Yan & Binlong Chen & Qingqing Yin & Zenghui Wang & Ye Yang & Fangjie Wan & Yaoqi Wang & Mingmei Tang & Heming Xia & Meifang Chen & Jianxiong Liu & Siling Wang & Qiang Zhang & Yiguang Wang, 2022. "Dissecting extracellular and intracellular distribution of nanoparticles and their contribution to therapeutic response by monochromatic ratiometric imaging," Nature Communications, Nature, vol. 13(1), pages 1-14, December.

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