Polyphenol-stabilized coacervates for enzyme-triggered drug delivery

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 and Jesse V. Jokerst ()
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Wonjun Yim: University of California San Diego
Zhicheng Jin: University of California San Diego
Yu-Ci Chang: University of California San Diego
Carlos Brambila: University of California San Diego
Matthew N. Creyer: University of California San Diego
Chuxuan Ling: University of California San Diego
Tengyu He: University of California San Diego
Yi Li: University of California San Diego
Maurice Retout: University of California San Diego
William F. Penny: University of California San Diego
Jiajing Zhou: University of California San Diego
Jesse V. Jokerst: University of California San Diego

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Stability issues in membrane-free coacervates have been addressed with coating strategies, but these approaches often compromise the permeability of the coacervate. Here we report a facile approach to maintain both stability and permeability using tannic acid and then demonstrate the value of this approach in enzyme-triggered drug release. First, we develop size-tunable coacervates via self-assembly of heparin glycosaminoglycan with tyrosine and arginine-based peptides. A thrombin-recognition site within the peptide building block results in heparin release upon thrombin proteolysis. Notably, polyphenols are integrated within the nano-coacervates to improve stability in biofluids. Phenolic crosslinking at the liquid-liquid interface enables nano-coacervates to maintain exceptional structural integrity across various environments. We discover a pivotal polyphenol threshold for preserving enzymatic activity alongside enhanced stability. The disassembly rate of the nano-coacervates increases as a function of thrombin activity, thus preventing a coagulation cascade. This polyphenol-based approach not only improves stability but also opens the way for applications in biomedicine, protease sensing, and bio-responsive drug delivery.

Date: 2024
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DOI: 10.1038/s41467-024-51218-8

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