Journal
JOURNAL OF COLLOID AND INTERFACE SCIENCE
Volume 603, Issue -, Pages 398-407Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2021.06.050
Keywords
DODAP; pH-responsive cationic nanocarriers; Self-assembly; SAXS; cryo-TEM; Antimicrobial peptide delivery
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Funding
- Swiss National Science Foundation [IZBRZ2_186251]
- Swiss National Science Foundation (SNF) [IZBRZ2_186251] Funding Source: Swiss National Science Foundation (SNF)
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The study shows that pH-responsive aminolipid self-assemblies can improve the targeted delivery of antimicrobial peptides. Through experiments, it was found that the pH-sensitive nanocarriers based on DODAP/water systems undergo colloidal transformations driven by the protonation of DODAP upon pH decrease. This knowledge can contribute to the design of future pH-responsive AMP delivery systems.
Hypothesis: pH-responsive aminolipid self-assemblies are promising platforms for the targeted delivery of antimicrobial peptides (AMPs), with the potential to improve their therapeutic efficiency and physico-chemical stability. Experiments: pH-sensitive nanocarriers based on dispersed self-assemblies of 1,2-dioleoyl-3-dimethylam monium-propane (DODAP) with the human cathelicidin LL-37 in excess water were characterized at different pH values using small-angle X-ray scattering, cryogenic transmission electron microscopy, and dynamic light scattering. Fluorescence and electrophoretic mobility measurements were used to probe the encapsulation efficiency of LL-37 and the nanocarriers' surface potential. Findings: Upon decreasing pH in the DODAP/water systems, normal oil-in-water emulsions at pH >= 5.0 transitioned to emulsions encapsulating inverse hexagonal and cubic structures at pH between 4.5 and 4.0, and mostly positively-charged vesicles at pH < 4.0. These colloidal transformations are driven by the protonation of DODAP upon pH decrease. The larger lipid-water interfacial area provided by the DODAP self-assemblies at pH <= 4.5 allowed for an adequate encapsulation efficiency of LL-37, favouring the formation of vesicles in a concentration-dependent manner. Contrary, LL-37 was found to dissociate from the emulsion droplets at pH 6.0. The knowledge on the pH-triggered self-assembly of LL-37 and DODAP, combined with the results on peptide release from the structures contribute to the fundamental understanding of lipid/peptide self-assembly. The results can guide the rational design of future pH-responsive AMP delivery systems. (C) 2021 The Author(s). Published by Elsevier Inc.
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