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Hydrogen-bonds mediate liquid-liquid phase separation of mussel derived adhesive peptides

Author

Listed:
  • Qi Guo

    (Nanyang Technological University (NTU))

  • Guijin Zou

    (Institute of High Performance Computing, A*STAR)

  • Xuliang Qian

    (Nanyang Technological University (NTU))

  • Shujun Chen

    (Nanyang Technological University (NTU))

  • Huajian Gao

    (Institute of High Performance Computing, A*STAR
    Nanyang Technological University (NTU))

  • Jing Yu

    (Nanyang Technological University (NTU)
    Nanyang Technological University (NTU))

Abstract

Marine mussels achieve strong underwater adhesion by depositing mussel foot proteins (Mfps) that form coacervates during the protein secretion. However, the molecular mechanisms that govern the phase separation behaviors of the Mfps are still not fully understood. Here, we report that GK-16*, a peptide derived from the primary adhesive protein Mfp-5, forms coacervate in seawater conditions. Molecular dynamics simulations combined with point mutation experiments demonstrate that Dopa- and Gly- mediated hydrogen-bonding interactions are essential in the coacervation process. The properties of GK-16* coacervates could be controlled by tuning the strength of the electrostatic and Dopa-mediated hydrogen bond interactions via controlling the pH and salt concentration of the solution. The GK-16* coacervate undergoes a pH induced liquid-to-gel transition, which can be utilized for the underwater delivery and curing of the adhesives. Our study provides useful molecular design principles for the development of mussel-inspired peptidyl coacervate adhesives with tunable properties.

Suggested Citation

  • Qi Guo & Guijin Zou & Xuliang Qian & Shujun Chen & Huajian Gao & Jing Yu, 2022. "Hydrogen-bonds mediate liquid-liquid phase separation of mussel derived adhesive peptides," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33545-w
    DOI: 10.1038/s41467-022-33545-w
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    References listed on IDEAS

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    1. Luigi Petrone & Akshita Kumar & Clarinda N. Sutanto & Navinkumar J. Patil & Srinivasaraghavan Kannan & Alagappan Palaniappan & Shahrouz Amini & Bruno Zappone & Chandra Verma & Ali Miserez, 2015. "Mussel adhesion is dictated by time-regulated secretion and molecular conformation of mussel adhesive proteins," Nature Communications, Nature, vol. 6(1), pages 1-12, December.
    2. Bartosz Gabryelczyk & Hao Cai & Xiangyan Shi & Yue Sun & Piet J. M. Swinkels & Stefan Salentinig & Konstantin Pervushin & Ali Miserez, 2019. "Hydrogen bond guidance and aromatic stacking drive liquid-liquid phase separation of intrinsically disordered histidine-rich peptides," Nature Communications, Nature, vol. 10(1), pages 1-12, December.
    3. Guokui Qin & Xiao Hu & Peggy Cebe & David L. Kaplan, 2012. "Mechanism of resilin elasticity," Nature Communications, Nature, vol. 3(1), pages 1-9, January.
    4. Tobias Priemel & Elena Degtyar & Mason N. Dean & Matthew J. Harrington, 2017. "Rapid self-assembly of complex biomolecular architectures during mussel byssus biofabrication," Nature Communications, Nature, vol. 8(1), pages 1-12, April.
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    Cited by:

    1. Wonjun Yim & Zhicheng Jin & Yu-Ci Chang & Carlos Brambila & Matthew N. Creyer & Chuxuan Ling & Tengyu He & Yi Li & Maurice Retout & William F. Penny & Jiajing Zhou & Jesse V. Jokerst, 2024. "Polyphenol-stabilized coacervates for enzyme-triggered drug delivery," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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